Microbial fuel cells (MFC) provide a new opportunity for simultaneous electricity generation and waste treatment. An improvement in the anode capacity of MFCs is essential for their scale-up and commercialization. In this work we demonstrate, for the first time, that plasma-based ion implantation could be used as an effective approach to modify carbon paper as an anode for MFC to improve its electricity-generating capacity. After the N(+) ion implantation, a decreased charge-transfer resistance is achieved, which is attributed to the increased C-N bonds after N(+) ion implantation. In addition, the surface roughness and hydrophobicity are also changed, which favor microbial adhesion on the anode surface. The cyclic voltammetry results show that both the electrochemical activity and the electron transfer are enhanced remarkably, leading to better MFC performance compared to the control. Such a plasma surface modification technique provides an effective way to modify the electrode for enhancing MFC performance for power generation.