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Magnesium‐based hydrogen storage material (MgH2) has attracted much attention due to its high hydrogen storage density (7.6 wt%). However, the high hydrogen dissociation enthalpy and slow hydrogen dissociation rate in bulk Mg hinder its wide application in the efficient hydrogen storage. In the present work, we study the hydrogen adsorption and desorption reactions of MgmHn (m = 1–6) nanoclusters...