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Continuous and effective hydrogen evolution under high current densities remains a challenge for water electrolysis owing to the rapid performance degradation under continuous large-current operation. In this study, theoretical calculations, operando Raman spectroscopy, and CO stripping experiments confirm that Ru nanocrystals have a high resistance against deactivation because of the synergistic adsorption of OH intermediates (OH
) on the Ru and single atoms. Based on this conceptual model, we design the Ni single atoms modifying ultra-small Ru nanoparticle with defect carbon bridging structure (UP-RuNi
/C) via a unique unipolar pulse electrodeposition (UPED) strategy. As a result, the UP-RuNi
/C is found capable of running steadily for 100 h at 3 A cm
, and shows a low overpotential of 9 mV at a current density of 10 mA cm
under alkaline conditions. Moreover, the UP-RuNi
/C allows an anion exchange membrane (AEM) electrolyzer to operate stably at 1.95 V
for 250 h at 1 A cm
.