The　preparation　of　stable　and　high-efficiency　heterogeneous　electro-Fenton　cathodes　for　the　treatment　of　pollutants　is　important　for　environmental　remediation.　Herein,　a　novel　N-doped　MOF-derived　Fe/Co　bimetallic　catalyst　was　in-situ　grown　on　graphite　felt　(GF)　surface　to　yield　a　composite　cathode　Fe/CoNHDC-400@GF　for　use　in　electro-Fenton　process.　The　introduction　of　cobalt　accelerated　electron　transfer　due　to　existing　polyvalent　metals.　The　synergistic　effect　between　Co0,　CoⅡ,　CoШ,　FeⅡ,　and　FeШ　enabled　the　continuous　generation　of　reactive　oxygen　species　(•OH　and　•O2−).　Under　near-neutral　conditions　(pH=6.5),　complete　removal　of　10　mg　L−1　chloroquine　phosphate　(CQP)　was　achieved　within　60　min.　Additionally,　efficient　removal　was　also　achievable　over　a　wide　pH　range　(pH=3–11).　The　mechanistic　investigations　indicated　•OH　as　a　major　active　oxygen　species　for　CQP　degradation.　A　combination　of　the　experimental　results　with　density　functional　theory　calculations　(DFT)　clarified　the　degradation　pathway　and　intermediate　products　of　CQP.　Moreover,　the　toxicity　of　degradation　products　significantly　reduced.　Overall,　valuable　insights　on　preparing　composite　cathodes　grown　in-situ　for　efficient　removal　of　refractory　pollutants　from　wastewater　during　the　heterogeneous　electro-Fenton　process　were　provided,　useful　for　future　consideration.　©　2024　Elsevier　Ltd