Abstract Developing highly efficient and durable electrocatalysts toward oxygen evolution reaction (OER) is an urgent demand to produce clean hydrogen energy. In this study, a series of medium‐entropy metal sulfides (MEMS) of (NiFeCoX) 3 S 4 (where X = Mn, Cr, Zn) are synthesized by a facile one‐pot solvothermal strategy using molecular precursors. Benefiting from the multiple‐metal synergistic effect and the low crystallinity, these MEMS show significantly enhanced electrocatalytic OER activity compared with the binary‐metal (NiFe) 3 S 4 and ternary‐metal (NiFeCo) 3 S 4 counterparts. Especially, (NiFeCoMn) 3 S 4 delivers a low overpotential of 289 mV at 10 mA cm −2 , a decent Tafel slope of 75.6 mV dec −1 and robust catalytic stability in alkaline medium, outperforming the costly IrO 2 benchmark electrocatalyst and the majority of the reported metal sulfide‐based electrocatalysts until now. These MEMS with facile synthesis and excellent electrocatalytic performance bring a great opportunity to design desirable electrocatalysts for practical application.