Indole is a high-toxic refractory nitrogen-containing compound that could cause serious harm to the human and ecosystem. It has been a challenge to develop economical and efficient technology for degrading indole. Microbial fuel cell (MFC) has great potential in the removal of organic pollutants utilizing microorganisms as catalysts to degrade organic matter into the nutrients. Herein, a novel anode of Fe2O3-polyaniline-dopamine hybrid composite modified carbon felt (Fe2O3-PDHC/CF) was prepared by electrochemical deposition. The degradation efficiency of indole by the MFC loading Fe2O3-PDHC/CF anode was up to 90.3 % in 120 h operation, while that of the MFC loading CF anode was only 44.0 %. The maximum power density of the MFC loading Fe2O3-PDHC/CF anode was 3184.4 mW·m-2, increasing 113 % compared to the MFC loading CF anode. The superior performances of the MFC with Fe2O3-PDHC surface-modified anode owned to the synergistic effect of high conductive Fe2O3 and admirably biocompatible polyaniline-dopamine. MFC with the Fe2O3-PDHC/CF anode could produce considerable electricity and effectively degrade indole in water, which demonstrated a practical approach for the efficient degradation of refractory organic compounds in wastewater.