Abstract: Bimetallic carbide Co/β-Mo₂C was prepared with the thermal treatment-assisted chemical method and used as an anode catalyst for Microbial Fuel Cells (MFCs). The morphology and content of Co/β-Mo₂C was studied with the scanning electron microscope (SEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS). Furthermore, the cyclic voltammetry (CV), the electrochemical impedance spectroscopy (EIS) and a single-chamber air-cathode Microbial Fuel Cell(MFC) were used to study the electrochemical performance of Co/β-Mo₂C. The results showed that due to the prominent electrochemical activity and excellent biocompatibility, the MFC device equipped with 3 mg/cm² Co/β-Mo₂C-decorated carbon paper anode delivered a power density of 483.3 mW/cm², and a coulomb efficiency of 3.7%, which are 1.30 and 1.68 times those of the pristine carbon paper anode MFCs respectively. This work provides a new path for the explorer of high-performance anodic catalysts for MFCs application.