Transition　metal　phosphides　(TMPs)　have　emerged　as　promising　alternatives　to　commercial　noble-metal-based　electrocatalysts　for　the　hydrogen　evolution　reaction　(HER).　However,　their　electrocatalytic　performance　is　still　far　from　practical　application.　Herein,　a　novel　self-supported　CoP-based　electrode　(MoZn-CoP/CC)　was　prepared,　in　which　Mo　and　Zn　co-doped　CoP　nanosheet　arrays　are　tightly　anchored　on　a　carbon　cloth　(CC)　matrix.　Remarkably,　the　as-prepared　MoZn-CoP/CC　electrode　exhibits　outstanding　HER　performance　with　exceptional　pH　universality.　More　importantly,　it　only　requires　modest　overpotentials　to　deliver　the　current　densities　exceeding　1.0 A cm−2　in　both　alkaline　and　acidic　media,　outperforming　the　commercial　Pt　catalyst.　Experimental　results　combined　with　theoretical　analysis　reveal　that　co-doping　of　Mo　and　Zn　can　modulate　the　electronic　structure　of　CoP,　thereby　optimizing　the　adsorption　energy　of　hydrogen　and　ultimately　improving　the　HER　performance.　This　work　provides　an　effective　strategy　to　tune　the　electronic　properties　of　TMPs　via　heteroatom　doping　for　enhancing　their　electrocatalytic　performance.　©　Youke　Publishing　Co.,　Ltd.　2025.