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The design and development of highly efficient electrocatalysts for oxygen evolution reaction (OER) are critical for renewable energy generation. Ni‐based electrocatalysts are widely used in the water electrolysis process. In this work, heterostructure consisting of selenides and layered double hydroxides (LDH) named (Co, Ni)Se4@NiFe‐LDH, are prepared by an LDH‐based strategy, in which the electronic structure of Ni active sites is regulated by interfacial electron interaction. The (Co, Ni)Se4@NiFe‐LDH shows an optimized charge distribution of Ni sites and excellent catalytic activity. The effective charge modulation results in lowering the energy barrier of OOH* intermediate formation and adequate adsorption strength of the intermediates on Ni‐active sites, which improves the kinetics of OER. Specifically, the (Co, Ni)Se4@NiFe‐LDH only requires an overpotential of 237 mV to reach the current density of 10 mA cm−2 under alkaline conditions. The results of this work demonstrate that reasonable engineering of heterostructure is an effective strategy to improve the intrinsic property of OER electrocatalysts for water splitting.