The design and manufacture of advanced anode materials with superior quality are significant for assembling high-performance microbial fuel cells (MFCs). The present study aims to investigate the synergistic effect of MoS2/CNTs nanocomposite as a novel anode-modifying material of MFCs. XRD, XPS, SEM, TEM and electrochemical analyses were performed to confirm the nanocomposite, to understand the morphology and to study the electrochemical properties of the modified electrodes. The performance of the MoS2/CNTs/carbon paper (CP)-MFCs was investigated and compared with that of MoS2/CP-MFCs, CNTs/CP-MFCs and CP-MFCs. The densest biofilm was formed on MoS2/CNTs-modified anode compared to MoS2/CP, CNTs/CP and CP anode, and MFCs with MoS2/CNTs-modified anodes achieved the maximum power density of 645 ± 32 mW m-2, which is three times greater than MFCs with bare carbon paper anodes (213 ± 10 mW m-2). These results demonstrate that the synthesized MoS2/CNTs nanocomposite could be exploited as an efficient anode catalyst for improving the performance of MFCs.