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Abstract A new photoelectrocatalytic (PEC) and microbial fuel cell (MFC) process was developed and applied to simultaneously remove refractory organic pollutants (i.e., phenol and aniline) from wastewater while recovering energy for in-situ utilization. The current generated by the MFC process was applied to drive the PEC reaction. Compared with single PEC or MFC processes, the PEC-MFC combined process showed higher pollutant and chemical oxygen demand (COD) removal capacities and electricity production. Over 95% of the phenol or aniline was removed by these process, even at high initial concentrations. The COD removal efficiencies for phenol and aniline were ca. 96% (from 700 to 29 mg L−1) and 70% (from 165 to 49 mg L−1), respectively. Although the PEC process showed a limited contribution to phenol and aniline removals (16.5% and 43%, respectively), the utilization of PEC-treated phenol or aniline streams resulted in a MFC with higher voltage output, higher coulombic efficiency, maximal volumetric power density, and lower internal resistance as compared to untreated water. High-performance liquid chromatography coupled with mass spectrometry measurements revealed quinones/hydroquinones and low molecular weight organic acids to be produced as intermediates after the PEC process, which could improve the production of electricity in the MFC. Highlights • A new process composed of photoelectrocatalysis (PEC) and microbial fuel cell (MFC) was developed. • PEC-MFC may simultaneously remove pollutants and recover energy for in-situ utilization. • The (hydro)Quinones and low-molecular-weight organic acid as products from PEC increase electricity production of MFC. • A consecutive, dynamic adsorption and degradation process in MFC supply stable current to drive PEC. [ABSTRACT FROM AUTHOR]