Self-Planarization of High-Performance Graphene Liquid Crystalline Fibers by Hydration

[Image: see text] Graphene fibers (GFs) are promising elements for flexible conductors and energy storage devices, while translating the extraordinary properties of individual graphene sheets into the macroscopically assembled 1D structures. We report that a small amount of water addition to the graphene oxide (GO) N-methyl-2-pyrrolidone (NMP) dispersion has significant influences on the mesophase structures and physical properties of wet-spun GFs. Notably, 2 wt % of water successfully hydrates GO flakes in NMP dope to form a stable graphene oxide liquid crystal (GOLC) phase. Furthermore, 4 wt % of water addition causes spontaneous planarization of wet-spun GFs. Motivated from these interesting findings, we develop highly electroconductive and mechanically strong flat GFs by introducing highly crystalline electrochemically exfoliated graphene (EG) in the wet-spinning of NMP-based GOLC fibers. The resultant high-performance hybrid GFs can be sewn on cloth, taking advantage of the mechanical robustness and high flexibility.