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Developing efficient, economical, and stable catalysts for the oxygen evolution reaction is pivotal for producing large-scale green hydrogen in the future. Herein, a vanadium-doped nickel-iron oxide supported on nickel foam (V-NiFe 2 O 4 /NF) is introduced, and synthesized via a facile hydrothermal method as a highly efficient electrocatalyst for water electrolysis. X-ray photoelectron and absorption spectroscopies reveal a synergistic interaction between the vanadium dopant and nickel/iron in the host material, which tunes the electronic structure of NiFe 2 O 4 to increase the number of electrochemically active sites. The V-NiFe 2 O 4 /NF electrode exhibited superior electrochemical performance, with a low overpotential of 186 mV at a current density of 10 mA cm -2 , a Tafel slope value of 54.45 mV dec -1 , and minimal charge transfer resistance. Employing the V-NiFe 2 O 4 /NF electrode as an anode in an alkaline anion exchange membrane water electrolyzer single-cell, a cell voltage of 1.711 V is required to achieve a high current density of 1.0 A cm -2 . Remarkably, the cell delivered an energy conversion efficiency of 73.30% with enduring stability, making it a promising candidate for industrial applications., (© 2025 Wiley‐VCH GmbH.)