The objective of this study is to assess bioelectricity generation, pollutant removal (COD, ammonium, nitrate) and the bacterial communities on anodes in constructed wetlands coupled with microbial fuel cells (CW-MFCs), through feeding the systems with three different types of synthetic wastewater (system 1: normal wastewater; system 2: ammonium-free wastewater; system 3: nitrate-free wastewater). Three CW-MFCs were operated with different wastewater concentrations and hydraulic retention times (HRTs) over a long time period (6 months). The results indicate that the maximum open circuit voltage (775.63 mV) and maximum power density (0.628 W m−3) were observed in system 3 (period 3), and that bioenergy production was inhibited in system 2, when feeding with ammonium-free wastewater continuously. COD removal rates in the three systems were similar during each period and ranged from 82.2 ± 6.8% to 98.3 ± 2.2%. Ammonium removal occurred at the air cathode of the CW-MFCs through nitrification, and a higher level of ammonium removal was found in system 1 (period 3) compared with the others. Meanwhile, denitrification occurred at the anaerobic anode of the CW-MFCs, and a large amount of nitrate was removed effectively. The highest nitrate removal rate was 98.8 ± 0.5% in system 2 (period 3). Additionally, four genera related to electricity generation were detected at the anode: Geothrix; Desulfovibrio; Desulfobulbus; and Geobacter. The relative abundances of Desulfovibrio, Desulfobulbus and Geothrix gradually increased during the three periods in system 3, which might be beneficial for bioelectricity generation. Further investigations are needed to optimize the CW-MFC performance and explain the mechanism behind the pollutant degradation and electron motion in the CW-MFCs.