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 MCu 0.10 -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 MCu 0.10 -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 MCu 0.10 -BNiMo. More importantly, industrial application of MCu 0.10 -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.