Comprehensive SummaryRealizing the hydrogen economy by water electrolysis is an attractive approach for hydrogen production, while the efficient and stable bifunctional catalysts under high current densities are the bottleneck that limits the half‐cell reactions of water splitting. Here, we propose an approach of hydrothermal and thermal annealing methods for robust MoO2/MoNi4@Ru/RuO2 heterogeneous cuboid array electrocatalyst with multiplying surface‐active sites by depositing a monolayer amount of Ru. Benefiting from abundant MoO2/MoNi4@Ru/RuO2 heterointerfaces on Cu foam, effectively driving the alkaline water splitting with superior hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). The synthesized MoO2/MoNi4@Ru/RuO2 has high HER activity, which realizes the working overpotentials of 48 mV at 50 mA cm‐2, further achieving overpotentials of 230 mV for industry‐level 1000 mA cm‐2 in alkaline water electrolysis. Moreover, it also showed an enhanced OER activity than commercial RuO2 with a small overpotential of 280 mV at 200 mA cm‐2 in alkaline media. When building an electrolyzer with electrodes of (‐)MoO2/MoNi4@Ru/RuO2IIMoO2/MoNi4@Ru/RuO2 (+), a cell voltage of 1.63 V, and 1.75 V just requires to support the current density of 200 mA cm‐2 and 500 mA cm‐2 in alkaline water electrolysis, much lower than the electrolyzer of (‐)Pt/CIIRuO2(+). This work demonstrates that MoO2/MoNi4@Ru/RuO2 heterogeneous nanosheet arrays are promising candidates for industrial water electrolysis applications, providing a possibility for the exploration of water electrolysis with a large current density.This article is protected by copyright. All rights reserved.