Abstract: | Despite nearly two decades of research, the absence of ideal, flexible, and transparent electrodes has been the biggest bottleneck for realizing flexible and printable electronics via roll‐to‐roll (R2R) method. A fabrication of poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate):graphene:ethyl cellulose (PEDOT:PSS:G:EC) hybrid electrodes by R2R process, which allows for the elimination of strong acid treatment. The high‐performance flexible printable electrode includes a transmittance (T) of 78% at 550 nm and a sheet resistance of 13 Ω sq?1 with excellent mechanical stability. These features arise from the PSS interacting strongly with the ethyoxyl groups from EC promoting a favorable phase separation between PEDOT and PSS chains, and the highly uniform and conductive G:EC enable rearrangement of the PEDOT chains with more expanded conformation surrounded by G:EC via the π–π interaction between G:EC and PEDOT. The hybrid electrodes are fully functional as universal electrodes for outstanding flexible electronic applications. Organic solar cells based on the hybrid electrode exhibit a high power conversion efficiency of 9.4% with good universality for active layer. Moreover, the organic light‐emitting diodes and photodetector devices hold the same level to or outperform those based on indium tin oxide flexible transparent electrodes. |