Ni3Mo3C was prepared by a modified organic colloid method and explored as anode catalyst for high-performance microbial fuel cell (MFC) based on Klebsiella pneumoniae (K. pneumoniae). The prepared sample was characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), and Brunauer-Emmett-Teller (BET). The activity of the sample as anode catalyst for MFC based on K. pneumoniae was investigated by cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and polarization curve measurement. The results show that the adding of nickel in Mo2C increases the BET surface area of Mo2C and improves the electrocatalytic activity of Mo2C towards the oxidation of microbial fermentation products. The power density of MFC with 3 mg cm(-2) Ni3Mo3C anode is far higher than that of the MFC with carbon felt as anode without any catalyst, which is 19 % higher than that of Mo2C anode and produced 62 % as much as that of Pt anode, indicating that Ni3Mo3C is comparative to noble metal platinum as anode electrocatalyst for MFCs by increasing the loading.