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© 2020 WILEY-VCH Verlag GmbH Co. KGaA, Weinheim.Metal-organic framework (MOF) is highly desirable as a functional material owing to its low density, tunable pore size, and diversity of coordination formation, but limited by the poor dielectric properties. Herein, by controlling the solvent and mole ratio of cobalt/linker, multidimension-controllable MOF-derived nitrogen-doped carbon materials exhibit tunable morphology from sheet-, flower-, cube-, dodecahedron- to octahedron-like. Tunable electromagnetic parameters of Co@N-doped ca