The development of efficient and durable high‐current‐density hydrogen production electrocatalysts is crucial for the large‐scale production of green hydrogen and the early realization of hydrogen economic blueprint. Herein, we have successfully driven the evolution of grain boundaries through Cu‐mediated NiMo bimetallic oxides (MCu‐BNiMo), which leading to the high efficiency of electrocatalyst for hydrogen evolution process (HER) in industrial‐grade current density. The optimal MCu0.10‐BNiMo demonstrated ultrahigh current density (> 2 A cm−2) at a smaller overpotential in 1 M KOH (572 mV), than that of BNiMo, which does not have lattice strain. Experimental and theoretical calculations revealed that MCu0.10‐BNiMo with optimal lattice strain generated more electrophilic Mo sites with partial oxidation owing to accelerated charge transfer from Cu to Mo, which lowers the energy barriers for H* adsorption. These synergistic effects led to the enhanced HER performance of MCu0.10‐BNiMo. More importantly, industrial application of MCu0.10‐BNiMo operated in alkaline electrolytic cell was also determined, with its current density reached 0.5 A cm−2 at 2.12 V and 0.1 A cm−2 at 1.79 V, which is nearly five‐fold that of the state‐of‐the‐art HER electrocatalyst Pt/C. Our strategy provides valuable insights for achieving industrial‐scale hydrogen production through a highly efficient HER electrocatalyst.This article is protected by copyright. All rights reserved