Methanol steam reforming (MSR) is a promising solution for achieving the integration of hydrogen storage, transportation, and in-situ supply. However, it is limited by the slow rate of hydrogen generation and low selectivity. This study constructed a highly active N-Cu/MoxC catalyst with strong interaction between Cu and MoxC, effectively enhancing methanol activation, hydrolysis, and hydrogen production efficiency. Under optimized condition, the 2.8 N-Cu/MoxC catalyst achieved a remarkable H2 productivity of 147.9 mmol gcat−1 h−1 and H2 selectivity of 65.7 %. N induced a partial transition from β-Mo2C phase to γ-MoC phase, resulting in a doubling of H2 production rate. The interfacial N-Cu-MoxC sites facilitated highly reactive efficient CH bond dissociation to convert CO+4H and OH activation, as well as the highly efficient CO reforming. Additionally, temperature programmed surface reaction and isotope testing futher coroborated its superiority in methanol dehydrogenation and hydrolysis dissociation. These discoveries can provide guidance for the design of advanced MSR catalysts.