Liquid crystalline assembled materials have been attracted a great deal of research attention as a promising new material with their high alignment which can result in outstanding performances. In recent years, graphene-based liquid crystalline fiber has arisen as a new carbonaceous fiber with high expectations in terms of both superior and functional performances. The property of graphene-based fiber depends on the fabrication process parameters such as spinning dope, post treatment. Therefore, the novel method to control each step is highly demanded for a wide application. We tried to develop the spinning dope with a new binder for a defect engineered fiber inspired by mussel adhesive polydopamine. By establishing two-step incorporating relying on surface polymerization and subsequent infiltration, we could address the intrinsic structural defect during fiber spinning process. This defect-controlled graphene fiber exhibited high mechanical strength and electrical conductivity simultaneously. In addition, we demonstrated a new-concept of graphene oxide reduction strategy using flash lamp annealing. Based on the spatial controllability of reduction level via anisotropic irradiation, the properties of fiber can be delicately counterbalanced to obtain optimized fiber for high sensitivity humidity sensors. Finally, we investigated graphene enabled superior performance actuator with multi-responsive to diverse external stimuli as a new fiber based application. The ratio of graphene and liquid crystal elastomer was carefully optimized, and actuation performance of composite fiber was measured under heat and light.