Zwitterionic Gradient Double-Network Hydrogel Membranes with Superior Biofouling Resistance for Sustainable Osmotic Energy Harvesting

Developing ion-selective membranes with anti-biofouling property and biocompatibility is highly crucial in harvesting osmotic energy in natural environments and for future biomimetic applications. However, the exploration of membranes with these properties in osmotic energy conversion remain largely unaddressed. Herein, a tough zwitterionic gradient double-network hydrogel membrane (ZGDHM) with excellent biofouling resistance and cytocompatibility for sustainable osmotic energy harvesting is demonstrated. The ZGDHM, composed of negatively charged 2-acrylamido-2-methylpropanesulfonic acid (AMPS) as the first scaffold network and zwitterionic sulfobetaine acrylamide (SBAA) as the second network, is prepared by a two-step photopolymerization, thus creating continuous gradient double-network nanoarchitecture and then remarkably enhanced mechanical properties. As verified by the experiments and simulations, the gradient nanoarchitecture endows the hydrogel membrane with apparent ionic diode effect and space-charge-governed transport property, thus facilitating directional ion transport. Consequently, the ZGDHM can achieve a power density of 5.44 W m⁻² by mixing artificial seawater and river water, surpassing the commercial benchmark. Most importantly, the output power can be promoted to an unprecedented value of 49.6 W m⁻² at the mixing of salt-lake water and river water, nearly doubling up most of the existing nanofluidic membranes. This study paves a new avenue toward developing ultrahigh-performance osmotic energy harvesters for biomimetic applications.     

Physical Double‐Network Hydrogel Adhesives with Rapid Shape Adaptability,Fast Self‐Healing,Antioxidant and NIR/pH Stimulus‐Responsiveness for Multidrug‐Resistant Bacterial Infection and Removable Wound Dressing

Developing physical double‐network (DN) removable hydrogel adhesives with both high healing efficiency and photothermal antibacterial activities to cope with multidrug‐resistant bacterial infection, wound closure, and wound healing remains an ongoing challenge. An injectable physical DN self‐healing hydrogel adhesive under physiological conditions is designed to treat multidrug‐resistant bacteria infection and full‐thickness skin incision/defect repair. The hydrogel adhesive consists of catechol–Fe³⁺ coordination cross‐linked poly(glycerol sebacate)‐co‐poly(ethylene glycol)‐g‐catechol and quadruple hydrogen bonding cross‐linked ureido‐pyrimidinone modified gelatin. It possesses excellent anti‐oxidation, NIR/pH responsiveness, and shape adaptation. Additionally, the hydrogel presents rapid self‐healing, good tissue adhesion, degradability, photothermal antibacterial activity, and NIR irradiation and/or acidic solution washing‐assisted removability. In vivo experiments prove that the hydrogels have good hemostasis of skin trauma and high killing ratio for methicillin‐resistant staphylococcus aureus (MRSA) and achieve better wound closure and healing of skin incision than medical glue and surgical suture. In particular, they can significantly promote full‐thickness skin defect wound healing by regulating inflammation, accelerating collagen deposition, promoting granulation tissue formation, and vascularization. These on‐demand dissolvable and antioxidant physical double‐network hydrogel adhesives are excellent multifunctional dressings for treating in vivo MRSA infection, wound closure, and wound healing.     

Self‐Supporting,Double Stimuli‐Responsive Porous Membranes From Polystyrene‐block‐poly(N,N‐dimethylaminoethyl methacrylate) Diblock Copolymers

Asymmetric membranes are prepared via the non‐solvent‐induced phase separation (NIPS) process from a polystyrene‐block‐poly(N,N‐dimethylaminoethyl methacrylate) (PS‐b‐PDMAEMA) block copolymer. The polymer is prepared via sequential living anionic polymerization. Membrane surface and volume structures are characterized by scanning electron microscopy. Due to their asymmetric character, resulting in a thin separation layer with pores below 100 nm on top and a macroporous volume structure, the membranes are self‐supporting. Furthermore, they exhibit a defect‐free surface over several 100 µm². Polystyrene serves as the membrane matrix, whereas the pH‐ and temperature‐sensitive minority block, PDMAEMA, renders the material double stimuli‐responsive. Therefore, in terms of water flux, the membranes are able to react on two independently applicable stimuli, pH and temperature. Compared to the conditions where the lowest water flux is obtained, low temperature and pH, activation of both triggers results in a seven‐fold permeability increase. The pore size distribution and the separation properties of the obtained membranes were tested through the pH‐dependent filtration of silica particles with sizes of 12–100 nm.     

Light‐Induced Swelling‐Responsive Conductive,Adhesive, and Stretchable Wireless Film Hydrogel as Electronic Artificial Skin

Light‐induced wireless soft electronic skin hydrogels with excellent mechanical and electronic properties are important for several applications, such as soft robotics and intelligent wearable devices. Precise control of reversible stretchability and capacitive properties depending on intermolecular interaction and surface characteristics remains a challenge. Here, a thin‐film hydrogel is designed based on titanium oxide (TiO₂) polydopamine–perfluorosilica carbon dot‐conjugated chitosan–polyvinyl alcohol‐loaded tannic acid with controllable hydrophobic–hydrophilic transition in the presence of UV–vis light irradiation. The shifting of surface wettability from hydrophobic to hydrophilic by irradiation affects thin‐film water permeability and swelling ratio. This allows the penetration of water into the matrix to change its mechanical strength, electronic properties, and adhesive behavior. Specifically, the hydrogel displays mechanical strain as high as 278% in response to light stimuli and demonstrates the ability to regain its initial state determining the elasticity of the fabricated material. Moreover, the thin‐film hydrogel shows an increase in conductivity to 1.096 × 10^?3 and 1.026 × 10^?3 S cm^?1 when irradiated with UV and visible light, respectively. The hydrogel exhibits capacitive reversibility that follows finger motion which can be identified directly or remotely using wireless connection, indicative of its possible applications as an artificial electronic skin.     

Ultra‐Thin Self‐Assembled Protein‐Polymer Membranes: A New Pore Forming Strategy

Self‐assembled membranes offer a promising alternative for conventional membrane fabrication, especially in the field of ultrafiltration. Here, a new pore‐making strategy is introduced involving stimuli responsive protein‐polymer conjugates self‐assembled across a large surface area using drying‐mediated interfacial self‐assembly. The membrane is flexible and assembled on porous supports. The protein used is the cage protein ferritin and resides within the polymer matrix. Upon denaturation of ferritin, a pore is formed which intrinsically is determined by the size of the protein and how it resides in the matrix. Due to the self‐assembly at interfaces, the membrane constitutes of only one layer resulting in a membrane thickness of 7 nm on average in the dry state. The membrane is stable up to at least 50 mbar transmembrane pressure, operating at a flux of about 21 000–25 000 L m^?2 h^?1 bar^?1 and displayed a preferred size selectivity of particles below 20 nm. This approach diversifies membrane technology generating a platform for “smart” self‐assembled membranes.     

Super Bulk and Interfacial Toughness of Physically Crosslinked Double‐Network Hydrogels

Conventional design wisdom prevents both bulk and interfacial toughness to be presented in the same hydrogel, because the bulk properties of hydrogels are usually different from the interfacial properties of the same hydrogels on solid surfaces. Here, a fully‐physically‐linked agar (the first network)/poly(N ‐hydroxyethyl acrylamide) (pHEAA, the second network), where both networks are physically crosslinked via hydrogen bonds, is designed and synthesized. Bulk agar/pHEAA hydrogels exhibit high mechanical properties (2.6 MPa tensile stress, 8.0 tensile strain, 8000 J m^?2 tearing energy, 1.62 MJ m^?3 energy dissipation), high self‐recovery without any external stimuli (62%/30% toughness/stiffness recovery), and self‐healing property. More impressively, without any surface modification, agar/pHEAA hydrogels can be easily and physically anchored onto different nonporous solid substrates of glass, titanium, aluminum, and ceramics to produce superadhesive hydrogel–solid interfaces (i.e., high interfacial toughness of 2000–7000 J m^?2). Comparison of as‐prepared and swollen gels in water and hydrogen‐bond‐breaking solvents reveals that strong bulk toughness provides a structural basis for strong interfacial toughness, and both high toughness mainly stem from cooperative hydrogen bonds between and within two networks and between two networks and solid substrates. This work demonstrates a new gel system to achieve superhigh bulk and interfacial toughness on nonporous solid surfaces.     

Novel Biocompatible Polysaccharide‐Based Self‐Healing Hydrogel

A novel biocompatible polysaccharide‐based self‐healing hydrogel, CEC‐l‐OSA‐l‐ADH hydrogel (“l” means “linked‐by”), is developed by exploiting the dynamic reaction of N‐carboxyethyl chitosan (CEC) and adipic acid dihydrazide (ADH) with oxidized sodium alginate (OSA). The self‐healing ability, as demonstrated by rheological recovery, macroscopic observation, and beam‐shaped strain compression measurement, is attributed to the coexistence of dynamic imine and acylhydrazone bonds in the hydrogel networks. The CEC‐l‐OSA‐l‐ADH hydrogel shows excellent self‐healing ability under physiological conditions with a high healing efficiency (up to 95%) without need for any external stimuli. In addition, the CEC‐l‐OSA‐l‐ADH hydrogel exhibits good cytocompatibility and cell release as demonstrated by three‐dimensional cell encapsulation. With these superior properties, the developed hydrogel holds great potential for applications in various biomedical fields, e.g., as cell or drug delivery carriers.     

Benzodithiophene Copolymer—A Low‐Temperature,Solution‐Processed High‐Performance Semiconductor for Thin‐Film Transistors

Poly(4,8‐didodecyl‐2,6‐bis‐(3‐methylthiophen‐2‐yl)‐benzo[1,2‐b:4,5‐b′]dithiophene) self‐assembled on appropriate substrates from solution and formed highly structured thin films at low temperatures. As an as‐prepared thin‐film semiconductor without thermal annealing, it exhibited excellent field‐effect transistor properties with mobility of ～ 0.15 cm² V^–1 s^–1 in thin‐film transistors.     

Self‐Assembly of Flexible Free‐Standing 3D Porous MoS2‐Reduced Graphene Oxide Structure for High‐Performance Lithium‐Ion Batteries

Flexible freestanding electrodes are highly desired to realize wearable/flexible batteries as required for the design and production of flexible electronic devices. Here, the excellent electrochemical performance and inherent flexibility of atomically thin 2D MoS₂ along with the self‐assembly properties of liquid crystalline graphene oxide (LCGO) dispersion are exploited to fabricate a porous anode for high‐performance lithium ion batteries. Flexible, free‐standing MoS₂–reduced graphene oxide (MG) film with a 3D porous structure is fabricated via a facile spontaneous self‐assembly process and subsequent freeze‐drying. This is the first report of a one‐pot self‐assembly, gelation, and subsequent reduction of MoS₂/LCGO composite to form a flexible, high performance electrode for charge storage. The gelation process occurs directly in the mixed dispersion of MoS₂ and LCGO nanosheets at a low temperature (70 °C) and normal atmosphere (1 atm). The MG film with 75 wt% of MoS₂ exhibits a high reversible capacity of 800 mAh g^?1 at a current density of 100 mA g^?1. It also demonstrates excellent rate capability, and excellent cycling stability with no capacity drop over 500 charge/discharge cycles at a current density of 400 mA g^?1.     

Anisotropic Hybrid Hydrogels with Superior Mechanical Properties Reminiscent of Tendons or Ligaments

Mimicking the hierarchically anisotropic structure and excellent mechanical properties of natural tissues, such as tendons and ligaments, using biomaterials is challenging. Despite recent achievements with anisotropic hydrogels, limitations remain because of difficulties in achieving both structural and mechanical characteristics simultaneously. A simple approach for fabricating hybrid hydrogels with a hierarchically anisotropic structure and superior mechanical properties that are reminiscent of tendons or ligaments is proposed. Alginate–polyacrylamide double‐network (DN) hydrogels incorporated with high aspect ratio mesoporous silica microparticles are stretched and fixed via subsequent drying and ionic crosslinking to achieve multiscale structures composed of an anisotropically aligned polymer network embedded with aligned microparticles. The mechanical properties of hydrogels can be further controlled by the degree of stretching, quantities, and functional groups of inorganic microparticles, and types of crosslinking cations. The subsequent reswelling results in a high water content (>80%) similar to that of natural tendons while high strength, modulus, and toughness are maintained. The optimized anisotropic hybrid hydrogel exhibits a tensile modulus of 7.2 MPa, strength of 1.3 MPa, and toughness of 1.4 MJ m^?3 even in the swollen state, which is 451‐, 27‐, and 2.2 times higher than that observed in the non‐swollen tough DN hydrogel. This study suggests a new strategy for fabricating anisotropic hydrogels with superior mechanical properties to develop new biomaterials for artificial tendons or ligaments.     

Ultrathin Polymer Films with Intrinsic Microporosity: Anomalous Solvent Permeation and High Flux Membranes

Organic solvent nanofiltration (OSN) membranes with ultrathin separation layers down to 35 nm in thickness fabricated from a polymer of intrinsic microporosity (PIM‐1) are presented. These membranes exhibit exceptionally fast permeation of n‐heptane with a rejection for hexaphenylbenzene of about 90%. A 35 nm thick PIM‐1 membrane possesses a Young's modulus of 222 MPa, and shows excellent stability under hydraulic pressures of up to 15 bar in OSN. A maximum permeance for n‐heptane of 18 Lm^?2h^?1bar^?1 is achieved with a 140 nm thick membrane, which is about two orders of magnitude higher than Starmem240 (a commercial polyimide‐based OSN membrane). Unexpectedly, decreasing the film thickness below 140 nm results in an anomalous decrease in permeance, which appears to be related to a packing enhancement of PIM‐1, as measured by light interferometry. Further, thermal annealing of the membranes formed from PIM‐1 reveals that their permeance is preserved up to temperatures in excess of 150 °C, whereas the permeance of conventional, integrally skinned, asymmetric polyimide OSN membranes decreases significantly when they are annealed under the same conditions. To rationalize this key difference in response of functional performance to annealing, the concept of membranes with intrinsic microporosity (MIMs) versus membranes with extrinsic microporosity (MEMs) is introduced.     

Green‐Chemical Synthesis of Ultrathin β‐MnOOH Nanofibers for Separation Membranes

Ultrathin β‐MnOOH nanofibers can be produced on a large scale via a green‐chemical method using an aqueous solution of very dilute Mn(NO₃)₂ and aminoethanol at room temperature. High‐magnification electron microscopy demonstrates that the β‐MnOOH nanofibers are 3–5 nm thin and up to 1 micrometer long and the nanofibers are parallel assembled into bundles with an average diameter of 25 nm. By a filtration process, ultrathin mesoporous membranes with strong mechanical, thermal, and chemical stabilities are prepared from the β‐MnOOH nanofiber bundles. The membranes can separate 10‐nm nanoparticles from water at a flux of 15120 L m^?2·h^?1·bar^?1, which was 2–3 times higher than that of commercial membranes with similar rejection properties. Based on the Young‐Laplace equation, β‐MnOOH nanofiber/polydimethylsiloxane composite membranes are developed through a novel downstream‐side evaporation process. From nanoporous to dense separation membranes can be achieved by optimizing the experimental conditions. The membranes show desirable separation performance for proteins, ethanol/water mixtures, and gases. The synthesis method of β‐MnOOH nanofibers is simple and environmentally friendly, and it is easily scalable for industry and applicable to other metal oxide systems. These composite membranes constitute a significant contribution to advanced separation technology.     

Stimuli‐Responsive Donor–Acceptor and DNA‐Crosslinked Hydrogels: Application as Shape‐Memory and Self‐Healing Materials

Carboxymethyl cellulose (CMC) chains are functionalized with self‐complementary nucleic acid tethers and electron donor or electron acceptor functionalities. The polymer chains crosslinked by the self‐complementary duplex nucleic acids and the donor–acceptor complexes as bridging units, yield a stiff stimuli‐responsive hydrogel. Upon the oxidation of the electron donor units, the donor–acceptor bridging units are separated, leading to a hydrogel of lower stiffness. By the cyclic oxidation and reduction of the donor units, the hydrogel is reversibly transformed across low and high stiffness states. The controlled stiffness properties of the hydrogel are used to develop shape‐memory hydrogels. In addition, CMC hydrogels crosslinked by donor–acceptor complexes and K⁺‐stabilized G‐quadruplexes reveal stimuli‐responsive properties that exhibit dually triggered stiffness functions. While the hydrogel bridged by the two crosslinking motifs reveals high stiffness, the redox‐stimulated separation of the donor–acceptor complexes or the crown‐ether‐stimulated separation of the G‐quadruplex bridges yields two alternative hydrogels exhibiting low stiffness states. The control over the stiffness properties of the dually triggered hydrogel is used to develop shape‐memory hydrogels, where the donor–acceptor units or G‐quadruplex bridges act as “memories”, and to develop triggered self‐healing process of the hydrogel.     

Mussel‐Inspired Contact‐Active Antibacterial Hydrogel with High Cell Affinity,Toughness, and Recoverability

Antibacterial hydrogel has received extensive attention in soft tissue repair, especially preventing infections those associated with impaired wound healing. However, it is challenging in developing an inherent antibacterial hydrogel integrating with excellent cell affinity and superior mechanical properties. Inspired by the mussel adhesion chemistry, a contact‐active antibacterial hydrogel is proposed by copolymerization of methacrylamide dopamine (MADA) and 2‐(dimethylamino)ethyl methacrylate and forming an interpenetrated network with quaternized chitosan. The reactive catechol groups of MADA endow the hydrogel with contact intensified bactericidal activity, because it increases the exposure of bacterial cells to the positively charged groups of the hydrogel and strengthens the bactericidal effect. MADA also maintains the good adhesion of fibroblasts to the hydrogel. Moreover, the hybrid chemical and physical cross‐links inner the hydrogel network makes the hydrogel strong and tough with good recoverability. In vitro and in vivo tests demonstrate that this tough and contact‐active antibacterial hydrogel is a promising material to fulfill the dual functions of promoting tissue regeneration and preventing bacterial infection for wound‐healing applications.     

Mechanical Properties of Robust Ultrathin Silk Fibroin Films

Robust ultrathin multilayer films of silk fibroin were fabricated by spin coating and spin‐assisted layer‐by‐layer assembly and their mechanical properties were studied both in tensile and compression modes for the first time. The ultrathin films were characterized by a high elastic modulus of 6–8 GPa (after treatment with methanol) with the ultimate tensile strength reaching 100 MPa. The superior toughness is also many times higher than that usually observed for conventional polymer composites (328 kJ m^–3 for the silk material studied here versus typical values of < 100 kJ m^–3). These outstanding properties are suggested to be caused by the gradual development of the self‐reinforcing microstructure of highly crystalline β‐sheets, serving as reinforcing fillers and physical crosslinks, a process that is well known for bulk silk materials but it is demonstrated here to occur in ultrathin films as well, despite their limited dimensions. However, the confined state within films thinner than the lengths of the extended domains causes a significantly reduced elasticity which should be considered in the design of nanosized films from silk materials. Such regenerated silk fibroin films with outstanding mechanical strength have potential applications in microscale biodevices, biocompatible implants, and synthetic coatings for artificial skin.     

A Synthetic Hydrogel Composite with the Mechanical Behavior and Durability of Cartilage

This article reports the first hydrogel with the strength and modulus of cartilage in both tension and compression, and the first to exhibit cartilage‐equivalent tensile fatigue strength at 100 000 cycles. These properties are achieved by infiltrating a bacterial cellulose (BC) nanofiber network with a poly(vinyl alcohol) (PVA)–poly(2‐acrylamido‐2‐methyl‐1‐propanesulfonic acid sodium salt) (PAMPS) double network hydrogel. The BC provides tensile strength in a manner analogous to collagen in cartilage, while the PAMPS provides a fixed negative charge and osmotic restoring force similar to the role of aggrecan in cartilage. The hydrogel has the same aggregate modulus and permeability as cartilage, resulting in the same time‐dependent deformation under confined compression. The hydrogel is not cytotoxic, has a coefficient of friction 45% lower than cartilage, and is 4.4 times more wear‐resistant than a PVA hydrogel. The properties of this hydrogel make it an excellent candidate material for replacement of damaged cartilage.     

Red‐ to NIR‐Emitting,BODIPY‐Based,K+‐Selective Fluoroionophores and Sensing Materials

Optical sensing materials for the selective measurement of potassium ions (K⁺) in water are presented. The indicator dyes are based on an aza‐crown ether as a receptor and borondipyrromethenes (BODIPY) dyes as fluorophores. Fluorescence enhancement is caused by the reduction of photoinduced electron transfer (PET) upon complexation with K⁺ ions. The family of new indicators possesses tuneable optical properties (green to red excitation, red to NIR emission) and PET efficiencies. They exhibit high brightness with quantum yields between 0.20 and 0.47 in the “on” state and a molar absorption coefficient between 30 000 and 290 000 m ^?1 cm^?1. The new indicator dyes are immobilized in biocompatible hydrogel matrices to obtain stable nonleaching and fast responding (t₉₀ ≈ 10 s) sensing materials for continuous measurements of potassium. They are realized in various formats such as planar optodes, fiber‐optic sensors, and water‐dispersible polymer‐based nanoparticles. Apart from fluorescence intensity measurements, self‐referenced read‐out of fluorescence decay time is demonstrated. All sensor materials display a high K⁺/Na⁺ selectivity and are not influenced by pH within the physiologically relevant range. Practical applicability of the materials is emphasized by application of a fiber‐optic sensor to quantification of K⁺ in serum, which shows excellent correlation with the reference measurements.     

Graphene‐Directed Supramolecular Assembly of Multifunctional Polymer Hydrogel Membranes

Polymer‐based nanoporous hydrogel membranes hold great potential for a range of applications including molecular filtration/separation, controlled drug release, and as sensors and actuators. However, to be of practical utility, polymer membranes generally need to be fabricated as ultrathin yet mechanically robust, have a large‐area yet be defect‐free and in some cases, their structure needs the capability to adapt to certain stimuli. These stringent and sometimes self‐conflicting requirements make it very challenging to manufacture such bulk nanostructures in a controllable, scalable and cost‐effective manner. Here, a versatile approach to the fabrication of multifunctional polymer‐based hydrogel membranes is demonstrated by a single step involving filtration of an aqueous dispersion containing chemically converted graphene (CCG) and a polymer. With CCG uniquely serving as a membrane‐ and pore‐forming directing agent and as a physical cross‐linker, a range of water soluble polymers can be readily processed into nanoporous hydrogel membranes through supramolecular interactions. With the interconnected CCG network as a robust and porous scaffold, the membrane nanostructure can easily be fine‐tuned to suit different applications simply by controlling the chemistry and concentration of the incorporated polymer. This work provides a simple and versatile platform for the design and fabrication of new adaptive supramolecular membranes for a variety of applications.     

A Novel Design Strategy for Fully Physically Linked Double Network Hydrogels with Tough,Fatigue Resistant,and Self‐Healing Properties

Double network (DN) hydrogels with two strong asymmetric networks being chemically linked have demonstrated their excellent mechanical properties as the toughest hydrogels, but chemically linked DN gels often exhibit negligible fatigue resistance and poor self‐healing property due to the irreversible chain breaks in covalent‐linked networks. Here, a new design strategy is proposed and demonstrated to improve both fatigue resistance and self‐healing property of DN gels by introducing a ductile, nonsoft gel with strong hydrophobic interactions as the second network. Based on this design strategy, a new type of fully physically cross‐linked Agar/hydrophobically associated polyacrylamide (HPAAm) DN gels are synthesized by a simple one‐pot method. Agar/HPAAm DN gels exhibit excellent mechanical strength and high toughness, comparable to the reported DN gels. More importantly, because the ductile and tough second network of HPAAm can bear stress and reconstruct network structure, Agar/HPAAm DN gels also demonstrate rapid self‐recovery, remarkable fatigue resistance, and notable self‐healing property without any external stimuli at room temperature. In contrast to the former DN gels in both network structures and underlying association forces, this new design strategy to prepare highly mechanical DN gels provides a new avenue to better understand the fundamental structure‐property relationship of DN hydrogels, thus broadening current hydrogel research and applications.     

Cucurbit[n]uril Supramolecular Hydrogel Networks as Tough and Healable Adhesives

Supramolecular noncovalent interactions are widely found in natural adhesion phenomena to control macroscopic adhesion and accomplish a variety of complex functions. Such supramolecular adhesives could impart the interfaces with intriguing properties, e.g., energy dissipation and self‐healing, on account of their dynamic nature. Here, we demonstrate that cucurbit[8]uril (CB[8])‐based supramolecular hydrogel networks can function as dynamic adhesives for diverse nonporous (e.g., glass, stainless steel, aluminum, copper, and titanium) and porous substrates (wood and bone). Without any surface prefunctionalization or introduction of curing agents, these CB[8] hydrogel networks can be readily applied by curing around the softening temperature, forming a tough and healable adhesive interlayer. The ability to fabricate a robust sandwich model consisting of substrate–CB[8] hydrogel network–substrate enables a number of applications including stretchable and wearable electronics, hybrid systems for biomedical devices or tissue/bone regeneration.