Abstract: | To overcome the drawbacks of solid microporous materials for CO2 capture, this proof‐of‐concept study demonstrates a low‐cost and rapid method for producing composites consisting of hypercrosslinked polymers (HCP) with a polyethyleneimine (PEI) binder. The resulting materials capture CO2 through physical and chemical absorption simultaneously. Compared with HCP, the composites exhibit higher CO2 uptake, higher volumetric density, and improved tolerance to water which is attributed to the PEI binder. |