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This invention discloses a nano-solid-state hydrogen storage material and its preparation method, belonging to the field of new energy materials technology. The nano-solid-state hydrogen storage material has a core-shell structure, comprising a nano-magnesium-based active phase core and a functionalized porous carbon material outer shell; the core contains in-situ grown multi-metal nanocatalyst particles; the outer shell is doped with non-metallic elements and loaded with metal-organic framework derivative nanoparticles; the core-shell structure is dispersed in a three-dimensional interconnected carbon-based network framework. The preparation method includes: preparing a multi-metal-organic framework precursor solution; synthesizing multi-metal-organic framework nanoparticles using a solvothermal method; chemically combining with a magnesium source and a nickel source to obtain a precursor composite; carbonization treatment to obtain a porous carbon-coated multi-metal nanocatalyst@magnesium-based composite material; constructing a three-dimensional network framework by combining with a functionalized carbon source and metal-organic framework derivatives; and high-pressure hydrogenation treatment. The material of this invention exhibits a low hydrogen desorption temperature, rapid hydrogen absorption and desorption kinetics, and excellent cycle stability.