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 anultra-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 mg