Efficient, stable, and scalable oxygen evolution reaction (OER) electrocatalysts are highly needed for industrial hydrogen production. Herein, MoFe-codoped NiS/Ni(OH) nanosheets with a sample size area of 200 cm are established on Ni foam via a facial hydrothermal method. It is found that Fe and MoO are effectively doped into the NiS/Ni(OH) nanosheets that are composed by heazlewoodite NiS and β-Ni(OH) nanocrystals. Based on the systematic study on the non-, Fe-, Mo-, and MoFe-doped NiS/Ni(OH) composites, it is revealed that Fe and MoO 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 η (263 mV) and η (301 mV), Tafel plot of 52 mV dec, 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.