LaF₃ was doped to the Mg(Al) solid solution alloy for enhancing the hydrogen absorption and desorption by ball milling. XRD was used to analyze the phases of the samples and the phase transition induced by hydrogenation and dehydrogenation. The microstructure and phase distribution were investigated by SEM and STEM. The hydrogen storage properties were measured by Sieverts method. For Mg_0.93Al_0.07-5wt.%LaF₃ nanocomposite, the hydrogen storage kinetic properties were significantly improved by reducing the hydriding and dehydriding activation energies to 65 and 78 kJ/mol, respectively, and the dehydriding enthalpy was calculated to be 69.7 kJ/mol. The improved hydrogen storage properties were mainly attributed to the catalytic effects of the in situ formed nanostructure Al₁₁La₃ and MgF₂ together with the dissolving of Al in Mg lattice.