Bifunctional　cathodes　have　attracted　widespread　interest　in　the　heterogeneous　electro-Fenton　(hetero-EF)　process.　In　this　study,　the　bifunctional　composite　cathode　co-modified　with　N-doped　carbon　CoFe　alloy　(CoFe@NC)　and　carbon　nanotubes　(CNTs),　designated　as　CoFe@NC-CNTs/CNTs/NF,　integrating　hydrogen　peroxide　(H2O2)　synthesis　and　catalysis,　was　prepared　for　efficient　degradation　of　atrazine　(ATZ)　under　the　near-neutral　condition　(pHi　=　5.9).　The　morphology　properties,　crystal　structure,　microstructures,　and　elemental　composition　were　determined.　The　influences　of　current　density,　initial　pH　value,　different　anions,　and　water　matrix　on　the　removal　of　ATZ　were　systematically　studied.　In　the　hetero-EF　process,　high　removal　efficiencies　of　ATZ　can　be　achieved　over　the　broad　pH　range　(3-9)　under　the　current　density　of　4.5　mA　cm-2.　The　removal　efficiency　of　ATZ　remained　at　90.2　+/-　0.3%　after　8　cycles　under　the　near-neutral　condition　(pHi　=　5.9).　Radical　quenching　tests　and　EPR　spectra　have　verified　that　both　free　radical　pathways　such　as　superoxide　anion　(O-2(center　dot-))　and　hydroxyl　radical　((OH)-O-center　dot)　and　non-radical　pathway　such　as　singlet　oxygen　(O-1(2))　contributed　to　ATZ　removal.　The　degradation　pathways　and　catalytic　mechanism　were　proposed.　Toxicity　evaluation　and　Escherichia　coli　growth　test　showed　that　the　toxicity　gradually　decreased　during　the　degradation　process.　This　work　provided　a　new　thought　for　developing　an　efficient　and　stable　bifunctional　cathode　to　construct　an　in-situ　hetero-EF　system　for　pollutants　removal　over　the　wide　pH　range.