Heterogeneous Electro-Fenton (EF) enables rapid elimination of recalcitrant organic pollutants without producing undesirable byproducts, but stable functioning of this process remains challenging. In this work, a porous composite of ferric oxide/nitrogen/carbon (Fe2O3/N-C) with good EF activity and stability was fabricated from iron-based metal-organic framework compounds (MOFs) and polyaniline via one-step pyrolysis. The incorporated Fe2O3 nanocrystals and the pyridinic and pyrrolic-N species endow the material with high catalytic activity for hydrogen peroxide (H2O2) generation and activation. The efficient degradation of bisphenol A and several other organic pollutants, dominated by a heterogeneous EF pathway, was achieved in acidic solution. The catalyst had low Fe leaching (0.52 mg/L after 2 h of reaction) and retained 98% of its original activity after four cycles of repeated use. Therefore, Fe2O3/N-C may serve as an efficient, stable, and environmentally benign heterogeneous EF catalyst for wastewater treatment and environmental remediation applications.