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Abstract: A simple and low‐cost fabrication method is needed to obtain effective and robust heterogeneous catalysts for the oxygen evolution reaction (OER). In this study, an electrocatalyst FeNiOxHy with a hierarchical structure is synthesized on nickel foam by a simple fabrication method through anion exchange from a metal phosphate to a metal hydroxide. The as‐fabricated FeNiOxHy electrode requires overpotentials of 206 and 234 mV to deliver current densities of 10 and 50 mA cm−2, respectively. The catalytic performance of FeNiOxHy is superior to that of most previously reported FeNi‐based catalysts, including NiFe layered double hydroxide. The catalyst also shows good long‐term durability at a current density of 50 mA cm−2 over 50 h with no activity decay under 1  m KOH. By comparison to the directly electrodeposited FeNi hydroxide in morphology and electrochemical properties, the improved activity of the catalyst could be mainly attributed to an enhancement of its intrinsic activity, which was caused by the anion exchange of phosphate to (oxy)hydroxide. Further studies by cyclic voltammetry indicated a stronger interaction between Ni and Fe from the negative shift of the oxidation peak of Ni2+/Ni3+ in comparison with reported FeNiOxHy, which promoted the generation of active Ni3+ species more easily. This work may provide a new approach to the simple preparation of effective and robust OER catalysts by anion exchange. [ABSTRACT FROM AUTHOR]