Binder-free NiO/MnO2-carbon felt electrode is prepared with a facile two-step hydrothermal method. The NiO self-grown on the carbon felt is used as the skeleton structure to support the in-situ growth of MnO2. Both the core and shell materials are excellent pseudocapacitance materials. The compositing of such pseudocapacitance metal oxides can produce synergistic effects, so that the modified electrode has a high capacitance. NiO/MnO2-carbon felt electrode also possesses a high specific surface area, super hydrophilicity and good biocompatibility, which are conducive to the enrichment of typical exoelectrogen Geobacter. As the anode, NiO/MnO2-carbon felt electrode can effectively improve the electricity generation and methyl orange (MO) wastewater degradation performances of microbial fuel cell (MFC). The highest output voltage and the maximum power density of MFC with NiO/MnO2-carbon felt anode are respectively 652 mV and 628 mW m(-2), which are much higher than those of MFC with MnO2-carbon felt anode (613 mV, 544 mW m(-2)), NiO carbon felt anode (504 mV, 197 mW M -2 ) and unmodified carbon felt anode (423 mV, 162 mW m(-2)). The decolourization efficiency and the chemical oxygen demand (COD) removal rate of MO for MFC with NiO/MnO2-carbon felt anode are respectively 92.5% and 58.2% at 48 h. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.