This article reports the discovery of chiral liquid crystals (CLCs) formed by graphene oxide (GO) sheets, which exhibit both lamellar and helical structures. The CLCs are characterized by their ability to form macroscopic fibers through wet-spinning, a method that overcomes the poor dispersibility of graphene. The fibers, made from GO sheets, are highly conductive and exhibit excellent mechanical properties, including high strength and elongation. The study also demonstrates the potential of these fibers in various applications, such as functional textiles and chemical sensors. The findings provide a new approach to fabricating high-performance carbon-based materials from natural graphite.This article reports the discovery of chiral liquid crystals (CLCs) formed by graphene oxide (GO) sheets, which exhibit both lamellar and helical structures. The CLCs are characterized by their ability to form macroscopic fibers through wet-spinning, a method that overcomes the poor dispersibility of graphene. The fibers, made from GO sheets, are highly conductive and exhibit excellent mechanical properties, including high strength and elongation. The study also demonstrates the potential of these fibers in various applications, such as functional textiles and chemical sensors. The findings provide a new approach to fabricating high-performance carbon-based materials from natural graphite.