The study experimentally investigates the changing performance of three-dimensional electrode H2O2-producting MFCs coupled with simultaneous wastewater treatment at various external cell voltages from 0.1 V to 0.8 V, in order to explore the optimal applied voltage and its reasons. The graphite particle electrodes made of graphite powders with polytetrafluoroethene (PTFE) as the binder are used as three-dimensional cathode. The results indicate that applied voltage is demonstrated to increase the productive rate and output of H2O2 and the efficiency of acetate degradation. Besides, a relatively high current density caused by a high applied voltage has a positive impact on anode performance in terms of organic degradation and coulombic efficiency. In addition, a relatively high voltage leads to the reduction of H2O2 and the evolution of H-2. Considering H2O2 concentration, anodic COD removal and current efficiencies of MFCs at various voltages, the optimal voltage is chosen to be 0.4 V, achieving the H2O2 generation of 705.6 mg L-1 at a rate of 2.12 kg m(-3) day(-1) and 76% COD removal in 8 h, with energy input of 0.659 kWh per kg H2O2. Coulombic efficiency, faradic efficiency and COD conversion efficiency are 92%, 96%, and 88% respectively. (C) 2015 Elsevier B.V. All rights reserved.