In article number 2002212, Jue Hu, Michael K. H. Leung, Bolong Huang, and co‐workers synthesize through the efficient interfacial engineering with transitional oxides, an earth‐abundant MoS2‐based catalyst. Owing to the optimized electroactive interfaces with efficient electron transfer, the efficient hydrogen evolution reaction (HER) in the alkaline is realized in MoS2/Ni2O3H with long‐term durability, providing a new strategy of developing superior catalysts for HER in the harsh alkaline environment.