Functional graphene-based fibers are promising as new types of flexible building blocks for the construction of wearable architectures and devices. Unique one-dimensional (1D) carbon nanotubes (CNTs) and 2D graphene (CNT/G) hybrid fibers with a large surface area and high electrical conductivity have been achieved by pre-intercalating graphene fibers with Fe3O4 nanoparticles for subsequent CVD growth of CNTs. The CNT/G hybrid fibers can be further woven into textile electrodes for the construction of flexible supercapacitors with a high tolerance to the repeated bending cycles. Various other applications, such as catalysis, separation, and adsorption, can be envisioned for the CNT/G hybrid fibers.