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Abstract 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⁻¹at 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 based on organic molecular‐modified rGO, the resulting hybrid device demonstrates an energy density of 74.7 W h kg⁻¹at a power density of 1.68 kW kg⁻¹while maintaining capacity retention of 91% after 10,000 cycles (20 A g⁻¹). The findings not only provide a promising electrode material for high‐performance hybrid capacitors but also open a new avenue toward knowledge‐based design of efficient electrode materials for other energy storage applications.