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Carbon-based materials were prepared to catalyze the V ^3+ /V ^2+ couple of vanadium redox flow battery using chitosan as the preliminary material and FeCl _3 as activating agent. Graphite microcrystals were the main structures of the obtained catalyst (CTS-Fe-900) activated by FeCl _3 , and they contained a large number of curled and overlapped carbon nanosheets. Compared with CTS-D-900 (without FeCl _3 as an activating agent), CTS-Fe-900 exhibits a better structure, higher graphitization degree, stronger current response, and smaller charge transfer resistance. The charge/discharge measurements indicates that the performances of the cell are improved by using the CTS-Fe-900-modified negative electrode in terms of increased discharge capacity and energy efficiency. Compared with pristine cell, the capacity retention for the CTS-Fe-900 modified cell maintains 82.2% at 50 mA cm ^−2 after 50 cycles, increased by 5.2%, and the corresponding energy efficiency reaches 81.3%, enhanced by 5.1%. This work reveals that CTS-Fe-900 catalyst can improve the comprehensive energy storage performance. The excellent electrocatalytic properties are mainly attribute to the effect of the FeCl _3 template and the increase in the degree of graphitization.