Abstract The development of efficient and durable noble metal‐free electrocatalyst for oxygen evolution reaction (OER) is highly desired in polymer electrolyte membrane (PEM) based water electrolysis and metal‐ air batteries but still remains a challenge. In this paper, we employ co‐precipitation method to prepare layered double hydroxides followed by calcination to synthesize nanoalloy catalyst, which was further characterized by X‐ray diffraction (XRD), scanning electron microscopy (SEM/EDS), high resolution transmission electron microscopy (HRTEM)and x‐ray photoelectron spectroscopy. As a novel OER electrocatalyst, the FeCoNi alloy catalyst shows remarkable OER activity enhancement with an overpotential of only 400 mV and a low Tafel slope 72 mV dec −1 . This work offers a unique paradigm for the synthesis of competitive electrocatalyst for OER with excellent durability under alkaline condition.