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The progress of highly efficient and stable nonprecious metallic-based electrocatalysts for the hydrogen evolution reaction (HER) in saline water/seawater is of great importance for the mass-scale production of hydrogen energy. Herein, a nanostructured NiFe-LDH/Cu2S heterostructure is constructed by growing NiFe-LDH nanosheets onto Cu2S nanorods. This heterostructure possesses exceptional HER performances with η10 = 36 mV (η10 indicates the overpotential at a current density of 10 mA cm2) and worked stably over 100 h in alkaline saline water. Moreover, the heterojunction catalyst acts as a bifunctional electrocatalyst for the anode and cathode, achieving a cell voltage of η10 = 1.463 V, which is superior to many reported electrocatalysts. The improvement of catalytic performance of NiFe-LDH/Cu2S can be ascribed to the charge redistribution on the heterointerface that accelerates the dissociation process caused by the formation of Ni with low electron cloud density. Moreover, the obtained covalent S–O bonds are beneficial to the adsorption of H*. In addition, NiFe-LDH/Cu2S also exhibits considerable catalytic performances in seawater electrolytes, delivering a cell voltage of η10 = 1.483 V with a stability of 27 h. We present a promising bifunctional electrocatalyst for water electrolysis in alkaline saline water/seawater which may find wide applications in the area of hydrogen energy.

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