<p>The development of non-noble electrocatalysts that simultaneously deliver exceptional activity, robust durability, and cost-effectiveness under industrial-grade current densities (&gt;1 A cm⁻²) remains a critical challenge for alkaline water electrolysis. Herein, we fabricate a heterostructured Co₃O₄-Fe₂O₃ electrocatalyst on carbon cloth via a scalable two-step synthesis strategy, demonstrating remarkable hydrogen evolution reaction performance in alkaline media. The optimized catalyst achieves ultra-low overpotentials of 119 mV and 1.0 V to reach current densities of 10 mA cm⁻² and 2 A cm⁻², respectively, accompanied by a near-unity Faradaic efficiency (99%). Notably, it maintains exceptional stability for 240 h at 2 A cm⁻². Density functional theory calculations reveal that strong interfacial electronic coupling between Co and Fe species facilitates rapid charge transfer and induces localized electron redistribution. This synergistic effect concurrently lowers the energy barriers for both H₂O dissociation and hydrogen product release at the Co active sites. Our work provides atomic-level insights into bimetallic electronic engineering, paving the way for designing high-performance electrocatalysts tailored for industrial hydrogen production.</p>