Activation　of　oxygen　over　non-precious　materials　has　been　an　imperative　task　to　develop　efficient　electrochemical　energy　storage　and　conversion　such　as　fuel　cells　and　metal-air　batteries.　Herein,　a　molten　salt　electrochemical　modulation　of　metal-nitrogen-carbon　based　compounds　(M–N–C)　is　achieved.　By　electrochemical　treatment　of　polydopamine-coated　NiCo2O4　(NiCo2O4@PDA)　in　molten　Li2CO3-Na2CO3-K2CO3　at　500　°C,　Ni/Co　bimetal-nitrogen-carbon　catalyst　(denoted　as　Ni/Co@NC)　consisting　of　Ni-Co　nanoparticles　anchoring　on　porous　nitrogen-doped　carbon　is　constructed　and　evaluated　as　electrocatalysts　towards　the　oxygen　reduction　reaction　(ORR).　Experimental　and　calculation　results　confirm　that　alloying　of　Ni-Co　and　nitrogen　doping　to　carbon　enhances　the　rate-determining　transformation　of　*OH　intermediate　during　ORR.　The　Ni/Co@NC　hence　shows　an　ORR　activity　comparable　with　the　commercial　Pt/C.　©　2022　Science　Press　and　Dalian　Institute　of　Chemical　Physics,　Chinese　Academy　of　Sciences