Herein, we aimed to obtain NiFe layered double hydroxide (LDH) with a controlled phase and surface morphology as a highly active and stable oxygen evolution catalyst via the electrochemical deposition method, which was thermodynamically stable for the oxygen evolution reaction (OER) in an alkaline medium. The NiFe-LDH sample was analyzed by sophisticated instruments and tested as an electrocatalyst on Toray carbon (TC). The NiFe-LDH electrocatalyst showed an excellent performance with lower overpotential of 0.27 V at 35 mA cm−2 and higher density of 125 mA cm−2 for OER in the 1 M KOH electrolyte solution. Moreover, the prepared catalyst exhibited unpredictable long-time stability for 700 h. From our knowledge, NiFe-LDH is a robust highly stable electrocatalyst compared to the recent reports. © 2022 by the authors.