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Three-dimensional (3D) nanostructures are commonly endowed with numerous active sites, large specific surface area, and good mechanical strength, which make them as an efficient candidate for energy storage and conversion. Herein, by considering the advantages of 3D nanostructures, we successfully fabricated carbon-coated nickel sulfide on a nickel foam (C@NS@NF) with a unique 3D treelike superstructure via a two-step hydrothermal process. By virtue of its hierarchical superstructures, 3D treelike architecture, and carbon shell encapsulation, the as-fabricated carbon-coated Ni 3 S 2 can be directly served as binder-free bifunctional electrodes for supercapacitor and hydrogen evolution reaction, where high specific areal capacitance (6.086 F cm -2 at 10 mA cm -2 ) for supercapacitors and low overpotential (92 mV at 10 mA cm -2 ) for the electrocatalyst have been demonstrated. These inspiring results of this material make it as a potential candidate for energy storage and conversion.