Exploring　nonprecious　electrocatalysts　for　water　splitting　with　high　efficiency　and　durability　is　critically　important.　Herein,　bimetallic　phosphides　are　encapsulated　into　graphitized　carbon　to　construct　a　C@NiCoP　composite　nanoarray　using　bimetallic　metal-organic　framework　(MOF)　as　a　self-sacrificial　template.　The　resulting　C@NiCoP　exhibits　superior　performance　for　pH-universal　electrocatalytic　hydrogen　evolution　reaction　(HER),　particularly　representing　a　low　overpotential　of　46.3　mV　at　10　mA　cm(-2)　and　Tafel　slope　of　44.1　mV　dec(-1)　in　alkaline　media.　The　structural　characterizations　combined　with　theoretical　calculation　demonstrate　that　tailored　electronic　structure　from　bimetal　atoms　and　the　synergistic　effect　with　graphitized　carbon　layer　could　jointly　optimize　the　adsorption　ability　of　hydrogen　on　active　sites　in　HER　process,　and　enhance　the　electrical　conductivity　as　well.　In　addition,　the　carbon　layer　served　as　a　protecting　shell　also　prevents　highly　dispersed　NiCoP　components　from　agglomeration　and/or　loss　in　harsh　media,　finally　improving　the　durability.　This　work　thus　provides　a　new　insight　into　optimizing　activity　and　stability　of　pH-universal　electrocatalysts　by　the　nanostructural　design　and　electronic　structure　modulation.　(C)　2021　Science　Press　and　Dalian　Institute　of　Chemical　Physics,　Chinese　Academy　of　Sciences.　Published　by　ELSEVIER　B.V.　and　Science　Press.　All　rights　reserved.