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The transfer of energy through hydrides is of particular significance in the biocatalysis field. In nature, some enzymes proceed the cascaded hydride transfers via nicotinamide adenine dinucleotide (NADH) with high selectivity in mild conditions. Moreover, chemical strategies are developed to transfer hydrides in vitro for NADH regeneration, which often require noble metals as mediators to promote the regioselectivity of NADH reduction to bioactive 1,4‐NADH. Recently, the Mo3+ hydride generated in amorphous molybdenum sulfide under cathodic potential can work for selective hydrogenation of NAD+ to 1,4‐NADH, opening promising prospects for sustainable biocatalysis.