Vacuum-assisted bilayer PEDOT:PSS/cellulose nanofiber composite film for self-standing, flexible, conductive electrodes

•PEDOT:PSS-CNF composite films were developed as a self-standing, highly flexible conductive film.•A simple vacuum-assisted filtration was used to fabricate a bilayer PEDOT:PSS-CNF film.•A bilayer PEDOT:PSS-CNF film exhibited good electrical conductivity and excellent flexibility. Sustainable cellulose nanofiber (CNF)-based composites as functional conductive materials have garnered considerable attention recently for their use in soft electronic devices. In this work, self-standing, highly flexible, and conductive PEDOT:PSS-CNF composite films were developed using a simple vacuum-assisted filtration method. Two different composite films were successfully fabricated and then tested: 1) a single-layer composite composed of a mixture of PEDOT:PSS and CNF phases and 2) a bilayer composite composed of an upper PEDOT:PSS membrane layer and a CNF matrix sub-layer. The latter composite was constructed by electrostatic/hydrogen bonding interactions between PEDOT:PSS and CNFs coupled with sequential vacuum-assisted filtration. Our results demonstrated that the resultant bilayer composite film exhibited a competitive electrical conductivity (ca. 22.6Scm−1) compared to those of previously reported cellulose-based composites. Furthermore, decreases in the electrical properties were not observed in the composite films when they were bent up to 100 times at an angle of 180° and bent multiple times at an angle of 90°, clearly demonstrating their excellent mechanical flexibility. This study provides a straightforward method of fabricating highly flexible, lightweight, and conductive films, which have the potential to be used in high-performance soft electronic systems.