In this work, a series of Ni/Co-MOFs with high specific capacitances were synthesized as anode materials using a one-step hydrothermal reaction method. NaOH in different amounts (3, 4, 5, and 6 mmol) was added during the synthesis to tune the pore structure of Ni/Co-MOFs. It was found that the Ni/Co-MOF-3 with a NaOH amount of 5 mmol exhibits the largest specific surface area and pore volume, which provides more active sites for the electrochemical reaction and facilitates ion diffusion at the interface of the electrolyte solution/active material, thus increasing the capacitance of the electrode material. The electrochemical test results show that the specific capacitance of Ni/Co-MOF-3 reaches 1361 F g