The　triggering　of　fast　hydrogen　spillover　through　regulating　the　charge　rearrangement　of　the　metal-support　serves　as　a　crucial　mechanism　for　decoupling　the　activity　of　HER　catalysts　from　the　adsorption　properties,　which　not　only　contributes　to　enhancing　the　performance　of　the　catalysts　but　also　facilitates　the　production　of　green　hydrogen.　Herein,　we　tailor　the　electronic　interaction　between　two-dimensional　(2D)　nitrogen-doped　MoC　(N-MoC)　nanosheets　and　an　ultra-low　content　of　Pt　nanoclusters　(1　wt%)　to　trigger　reverse　hydrogen　spillover　and　modulate　the　electronic　structure　of　Pt,　thus　achieving　efficient　and　stable　HER.　Compared　to　Pt/C　(0.229　A　mgPt-1),　Pt/N-MoC　demonstrates　a　mass　activity　of　12.945　A　mgPt-1,　representing　an　enhancement　of　nearly　57.5　times.　Notably,　the　excellent　electrocatalytic　performance　was　verified　in　the　proton　exchange　membrane　water　electrolyzer　configuration.　Combining　experimental　and　theoretical　analysis,　an　ultra-low　load　of　Pt　nanocluster　(1　wt%)　integrated　with　N-MoC　nanosheets　can　induce　a　charge　transfer　from　N-MoC　to　Pt,　thus　modulating　the　d-band　center　of　Pt　to　improve　the　hydrogen　adsorption　properties　and　achieving　fast　hydrogen　desorption　(Delta　G　=　0.019　eV);　furthermore,　a　small　difference　in　work　function　between　Pt　nanoclusters　and　the　N-MoC　were　achieved　to　dilute　charge　accumulation　between　the　metal-support　interface,　thus　reducing　the　energy　barrier　of　hydrogen　spillover.