Chirally Reversed Graphene Oxide Liquid Crystals

Colloidal liquid crystals (LCs) formed by nanoparticles hold great promise for creating new structures and topologies. However, achieving highly ordered hierarchical architectures and stable topological configurations is extremely challenging, mainly due to the liquid‐like fluidity of colloidal LCs in nature. Herein, an innovative synchronous nanofluidic rectification (SNR) technique for generating ultralong graphene oxide (GO) liquid crystal (GOLC) fibers with hierarchical core‐skin architectures is presented, in which the GO sheet assemblies and hydrogel skin formation are synchronous. The SNR technique conceptually follows two design principles: horizontal polymer‐flow promotes the rapid planar alignment of GO sheets and drives the chiral‐reversing of cholesteric GOLCs, and in situ formed hydrogel skin affords some protection against environmental impact to maintain stable topological configurations. Importantly, the dried fibers retain the smooth surface and ordered internal structures, achieving high mechanical strength and flexibility. The linear and circular polarization potential of GOLC fibers are demonstrated for optical sensing and recognition. This work may open an avenue toward the scalable manufacture of uniform and robust, yet highly anisotropic, fiber‐shaped functional materials with complex internal architectures.