Efficient, stable, and scalable oxygen evolution reaction (OER) electrocatalysts are highly needed for industrial hydrogen production. Herein, MoFe‐codoped Ni3S2/Ni(OH)2 nanosheets with a sample size area of 200 cm2 are established on Ni foam via a facial hydrothermal method. It is found that Fe3+ and MoO42− are effectively doped into the Ni3S2/Ni(OH)2 nanosheets that are composed by heazlewoodite Ni3S2 and β‐Ni(OH)2 nanocrystals. Based on the systematic study on the non‐, Fe‐, Mo‐, and MoFe‐doped Ni3S2/Ni(OH)2 composites, it is revealed that Fe3+ and MoO42− play important roles in reducing the interfacial charge transfer and increasing the electrochemical active surface area, respectively. When doping at a MoFe molar ratio of 5/3, the synergistic effect of Fe and Mo leads to an optimum OER property with low overpotentials of η100 (263 mV) and η500 (301 mV), Tafel plot of 52 mV dec−1, and long durability for at least 24 h. An effective strategy for high‐efficiency, long‐durability, and nonprecious OER electrocatalysts with promising applications is provided.