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In recent years, the use of selected additives for improving the kinetic behavior of the system 2LiH + MgB₂ (Li-RHC) has been investigated. As a result, it has been reported that some additives (e.g., 3TiCl₃·AlCl₃), by reacting with the Li-RHC components, form nanostructured phases (e.g., AlTi₃) possessing peculiar microstructural properties capable of enhancing the system’s kinetic behavior. The effect of in-house-produced AlTi₃ nanoparticles on the hydrogenation/dehydrogenation kinetics of the 2LiH + MgB₂ (Li-RHC) system is explored in this work, with the aim of reaching high hydrogen storage performance. Experimental results show that the AlTi₃ nanoparticles significantly improve the reaction rate of the Li-RHC system, mainly for the dehydrogenation process. The observed improvement is most likely due to the similar structural properties between AlTi₃ and MgB₂ phases which provide an energetically favored path for the nucleation of MgB₂. In comparison with the pristine material, the Li-RHC doped with AlTi₃ nanoparticles has about a nine times faster dehydrogenation rate. The results obtained from the kinetic modeling indicate a change in the Li-RHC hydrogenation reaction mechanism in the presence of AlTi₃ nanoparticles.