Nanoengineered NiFe Anode Sustains 100 Hours Stability at Industrial‐Grade Current Density of 500 mA/cm ² at Low Overpotential

ABSTRACT Industrial hydrogen production via water electrolysis is critically limited by the oxygen evolution reaction (OER), especially at high current densities (>500 mA cm −2 ) where conventional NiFe electrocatalysts fail due to poor conductivity and mass transport. We overcome this barrier through a transformative nanoengineering strategy, namely, of boron‐doped, mesoporous NiFe alloy nanosheets directly grown on carbon cloth (m‐NiFe‐CC). This approach uniquely leverages dimethylamine borane as a dual reducing agent/boron dopant and Brij 56 surfactant to create ordered 5–7 nm mesopores, enabling efficient mass/charge transport. The optimized m‐NiFe‐CC achieves record‐low overpotentials of 225, 270, and 329 mV at 10, 100, and 500 mA cm −2 outperforming state‐of‐the‐art NiFe catalysts, while exhibiting an 8‐fold higher turnover frequency (0.7 s −1 at 300 mV) and exceptional 100‐h stability at industrial‐grade current density. In situ surface reconstruction forms conductive NiFeB cores and active NiFeOOH phases, driven by boron‐mediated electronic modulation. This work establishes a scalable paradigm for nanoscale architectural control in high‐current‐density electrocatalysis, bridging fundamental innovation with industrial green hydrogen production.