Electrochemical splitting of water is an efficient pathway to the energy revolution. The challenge of balancing excellent electrochemical performance with the high cost of existing hydrogen evolution reaction catalysts has forced the development of efficient non-noble metal catalysts. Here, we prepared a FeCoNiWMo high-entropy alloy having a rhomboidal structure with atomic random occupancy. The unique atomic random occupation facilitates the formation of a self-circulating adsorption–desorption structure with fast electron transport inside, which significantly promotes water splitting. Especially, the overpotential of the catalyst at a current density of 10 mA cm–2 is only 35 mV under alkaline conditions. This work emphasizes the importance of coordinating a self-circulating proton transport structure and a disordered high-entropy state to manipulate the adsorption energy of an intermediate for developing high-performance electrocatalysts.

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