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HighlightsThree types of Ni 3 Si 2  were successfully fabricated by low-pressure all-solid melting-reconstruction chemical vapor deposition, and the growth pattern changed with the carbon source content.    In a carbon-rich atmosphere, high-energy atoms bombard the Ni and Si surface, and reduce the free energy in the solid Ni–Si particles’ thermodynamic equilibrium, considerably catalyzing the growth of Ni–Si nanocrystals.    Ni 3 Si 2 /NiOOH/graphene provides a large specific area and NiOOH inhibits insulation on the electrode surface in an alkaline solution and accelerates the electron exchange rate.Electronic supplementary material  The online version of this article (10.1007/s40820-020-00527-w) contains supplementary material, which is available to authorized users.

Superior Pseudocapacitive Storage of a Novel Ni3Si2/NiOOH/Graphene Nanostructure for an All-Solid-State Supercapacitor