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It is a great challenge to induce the formation of the RuP4 phase and realize the construction of a metal‐rich phase/phosphorus‐rich phase‐ruthenium phosphide heterostructure by directional regulation of the proportion of P and metal atoms. The ultra‐high conductivity of Ru2P and the excellent ability of V‐doped RuP4 to absorb/desorb H* are confirmed by density functional theory (DFT) calculations, which laid a theoretical foundation for the construction of a unique Ru2P/V‐RuP4 structure to accelerate HER reaction kinetics. This work innovatively uses the V‐doping strategy to induce the formation of RuP4 phase with high intrinsic activity, and finally construct V‐RuxPy nanosheets with rich Ru/Ru2P/V‐RuP4 heterostructures. Thanks to the rich Ru/Ru2P/V‐RuP4 heterostructure and the optimization of V dopants, the V‐RuxPy catalyst only needs 180 mV to obtain an industrial‐grade current density of 1 A cm−2. In summary, this work provides a new idea for the design and performance optimization of ruthenium‐based catalysts. [ABSTRACT FROM AUTHOR]

Platinum (Pt)‐based compounds are the benchmarked catalysts for hydrogen evolution reaction (HER) but exhibit slow kinetics in alkaline environments. The *OH accumulation on Pt surface can block active sites, affecting proton reduction and water re‐adsorption. Alloying Ruthenium (Ru) with Pt sites can significantly modulate the adsorption and desorption of water dissociation intermediates. Choosing suitable supports and utilizing metal‐support interaction (MSI) is crucial for active site optimization. PtRu alloy anchored on tungsten oxide (WO3) with rich oxygen vacancies (OV) is prepared through an ultrafast microwave‐assisted approach. Benefiting from the coupling effects between alloying and MSI, PtRu/WO3‐OV exhibits exceptionally high HER activity. In 1 m KOH, 1 m KOH + seawater, and 0.5 m H2SO4, it requires ultralow overpotentials of 9, 26, and 6 mV to achieve 10 mA cm−2, respectively. The designed catalyst surpasses commercial Pt/C in mass activity and demonstrates considerable potential for intermittent energy integration. Density functional theory reveals that alloying Ru with Pt sites significantly reduces the energy barrier of dissociating *OH, modulating blockage on the surface and then promoting the overall alkaline HER process. This study offers insights into the rapid synthesis of non‐carbon supported catalysts with Pt site modulation for alkaline hydrogen generation. [ABSTRACT FROM AUTHOR]