Two essential characteristics that are required for hybrid electrocatalysts to exhibit higher oxygen and hydrogen evolution reaction (OER and HER, respectively) activity are a favorable electronic configuration and a sufficient density of active sites at the interface between the two materials within the hybrid. In the present study, a hybrid electrocatalyst is introduced with a novel architecture consisting of coral‐like iron nitride (Fe2N) arrays and tungsten nitride (W2N3) nanosheets that satisfies these requirements. The resulting W2N3/Fe2N catalyst achieves high OER activity (268.5 mV at 50 mA cm−2) and HER activity (85.2 mV at 10 mA cm−2) with excellent long‐term durability in an alkaline medium. In addition, density functional theory calculations reveal that the individual band centers experience an upshift in the hybrid W2N3/Fe2N structure, thus improving the OER and HER activity. The strategy adopted here thus provides a valuable guide for the fabrication of cost‐effective multi‐metallic crystalline hybrids for use as multifunctional electrocatalysts.

Perovskite oxides with exsolved metal nanoparticles recently attract great attention because of their outstanding activity and stability at elevated temperature. Despite many pioneering works on catalyst development, the underline mechanism...