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The introduction of composite components to construct heterointerfaces is an important way to improve the electrocatalytic performance of materials. However, selecting appropriate components to accelerate the elementary reaction rates of the hydrogen evolution reaction (HER) in alkaline media is still in challenge. Here, a Ni‐CeF3‐VN multi‐component material is successfully constructed, which exhibits excellent HER catalytic activity (33 mV at 10 mA cm−2). The experimental and computational results show that the Ni‐VN and Ni‐CeF3 dual heterointerfaces can effectively promote the transfer of OH− adsorption site from Ni to VN and optimize the adsorption energy of intermediate H respectively, which together accelerate the rate of the multi‐step hydrogen evolution reaction in alkaline solution and thus lead to a significantly improved HER performance compared to the pure Ni. Furthermore, the solar to hydrogen (STH) efficiency can reach 10.34%. This work provides an effective guide for the design of high‐efficiency multicomponent materials in the future. [ABSTRACT FROM AUTHOR]