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This invention relates to a magnesium-based composite hydrogen storage material regulated by UiO-66, its preparation method, and its application. The high-performance magnesium-based composite hydrogen storage material provided comprises MgH2 and UiO-66, wherein MgH2 powder is the main phase, and UiO-66 is a high-temperature resistant metal-organic framework (MOF) composed of Zr, O, and C, possessing a large specific surface area and ultra-high structural stability, and plays a catalytic role. It is synthesized by hydrothermal and calcination methods. Compared with existing technologies, the magnesium-based composite hydrogen storage material provided by this invention has a dehydrogenation temperature range of 180 ℃–271 ℃ and a dehydrogenation activation energy as low as 69.26 kJ / mol. ‑1 It also possesses rapid room-temperature hydrogen absorption capacity and excellent circulating hydrogen storage performance, which is of great significance for promoting the application of MgH2 and improving its hydrogen storage performance.