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Compact, light, and powerful energy storage devices are urgently needed for many emerging applications; however, the development of advanced power sources relies heavily on advances in materials innovation. Here, the findings in rational design, one‐pot synthesis, and characterization of a series of Ni hydroxide‐based electrode materials in alkaline media for fast energy storage are reported. Under the guidance of density functional theory calculations and experimental investigations, a composite electrode composed of Co‐/Mn‐substituted Ni hydroxides grown on reduced graphene oxide (rGO) is designed and prepared, demonstrating capacities of 665 and 427 C g⁻¹ at current densities of 2 and 20 A g⁻¹, respectively. The superior performance is attributed mainly to the low deprotonation energy and the facile electron transport, as elaborated by theoretical calculations. When coupled with an electrode …