In　sulfate　radical-based　advanced　oxidation　processes　(SR-AOPs),　high-efficiency　and　perdurable　materials　have　drawn　considerable　interest　for　use　as　cathodes,　which　can　effectively　degrade　refractory　organic　contaminants　through　the　synergistic　electro-activation　and　transition　metal　activation　of　persulfate　(PS).　Here,　the　FeCuO@C　modified　composite　cathode　(FeCuO@C/AGF)　was　synthesized　via　the　solvothermal　and　thermal　treatment　method　based　on　the　CuFe-MOF-74　structure,　and　the　electro-activation　PS　process　(EC/FeCuO@C/AGF/PS)　was　developed　to　effectively　remove　atrazine　(ATZ).　The　surface　morphology,　electrochemical　characteristics,　chemical　composition,　crystal　structure,　and　electrode　surface　wettability　of　FeCuO@C/AGF　were　investigated.　It　was　found　that　the　proposed　EC/FeCuO@C/AGF/PS　process　can　successfully　remove　100%　of　ATZ　in　20　min　at　a　low　current　density　(2　mA　cm−2)　and　a　low　PS　concentration　(0.4　mM),　and　PS　is　successfully　activated　by　combining　the　electrical　and　transition　metal　synergistic　activation.　The　FeCuO@C/AGF　cathode　exhibits　outstanding　catalytic　functionality　over　a　broad　pH　range　(2–9)　and　remains　stable　over　five　successive　cycles.　Additionally,　the　active　species　involved　in　the　reaction　as　well　as　the　potential　ATZ　degradation　reaction　mechanisms　and　pathways　are　discussed.　Electrochemical　oxidation　is　a　process　in　which　both　radicals　(SO4·−,　·OH,　and　O2·−)　and　non-radical　(1O2)　participate　in　the　degradation　of　ATZ.　The　intermediates　of　the　ATZ　degradation　process　were　studied　upon　the　toxicity　changing,　and　the　toxicity　of　the　intermediates　was　found　to　be　reduced　during　degradation.　These　results　present　a　novel　approach　toward　the　establishment　of　an　effective　and　reliable　electrode　in　SR-AOPs　that　can　efficiently　treat　pesticide　wastewater.　©　2023　Elsevier　Ltd