Granular activated carbon (GAC) has been widely used at the anode of a microbial fuel cell (MFC) to enhance anode performance due to its outstanding capacitance property. To the best of our knowledge, there haven't been any studies on GAC in the cathode for biofilm development and nitrate reduction in MFC. In this study, by adding GAC to biocathode, we investigated the impact of different GAC amounts and stirring speeds on power generation and nitrate reduction rate in MFC. The denitrification rate was found to be nearly two-times higher in MFCs with GAC (0.046 ± 0.0016 kg m−3 d−1) compared to that deprived of GAC (0.024 ± 0.0012 kg m−3 d−1). The electrotrophic denitrification has produced a maximum power density of 37.6 ± 4.8 mW m−2, which was further increased to 79.2 ± 7.4 mW m−2 with the amount of GAC in the biocathode. A comparative study performed with chemical catalyst (Pt carbon with air sparging) cathode and GAC biocathode showed that power densities produced with GAC biocathode were close to that with Pt cathode. Cyclic voltammetry analysis conducted at 10 mV s−1 between −0.9 V and +0.3 V (vs. Ag/AgCl) showed consistent reduction peaks at −0.6V (Ag/AgCl) confirming the reduction reaction in the biocathode. This demonstrates that the GAC biocathode used in this research is effective at producing power density and denitrification in MFC. Our belief that the nitrate reduction was caused by the GAC biocathode in MFC was further strengthened when SEM analysis showing bacterial aggregation and biofilm formation on the surface of GAC. The GAC biocathode system described in this research may be an excellent substitute for MFC's dual functions of current generation and nitrate reduction.