Pollution by perfluorooctanoic acid (PFOA), a highly persistent and toxic substance, is commonly addressed with several approaches, but the need for post-treatment affects their environmental and economic sustainability. Biodegradation, which can efficiently degrade micropollutants in water under optimal conditions, offers a promising solution, but faces challenges from the persistence of the C-F bond and the high reactivity of F-. Despite recent use of various microorganisms for PFOA degradation, performance issues persist. In this study, we aimed to simulate PFOA degradation while mixed culture anammox granules oxidize NH4+ and to confirm the effects of electric potential and Fe(Ⅲ) applications on PFOA degradation. A control reactor containing only anammox granules exhibited NH4+ and PFOA removal efficiencies of 11.52% and 19.2%, respectively, with traceable biodegradation at 3.7%. In contrast, a reactor that applied both electric potential and Fe(Ⅲ) demonstrated enhanced removal efficiencies of 41.98% and 50.93%, with traceable biodegradation at 35.03%. Bio-electrochemical properties also improved, showing an average current generation of 331.95 μA and Coulombic efficiency of 141.79 ± 7.6%. This study shows that mixed-culture anammox granules with electric potential and Fe(Ⅲ) can be introduced for efficient PFOA biodegradation and provides the basis for further studies on overcoming the limitations of PFOA biodegradation.