As a kind of carbonaceous materials with high mechanical strength, carbon fiber is traditionally used as the electrode for structural batteries due to its high electric conductivity. However, the structural batteries based on carbon fiber reinforced polymer composites (CFRP) mainly suffer from two disadvantages of moderate interfacial properties due to low wettability for most polymers and limited capacity during charge/discharge. Therefore, carbon fiber modification which can enhance the properties of CFRP mechanically and electrochemically is in high demand. Herein, we report on a kind of carbon fiber which is modified by MOF nanosheets and embraces high potential to be used as electrode for structural batteries in replacement of pristine carbon fiber.