To improve the hydrogen storage performance, Mg₃La alloy and TiCl₃ is ball milled simultaneously with LiBH₄ to yield a designed composition. It has been revealed that there is a synergistic effect of Mg₃La alloy and TiCl₃ on the dehydrogenation of LiBH₄, which improves the dehydrogenation performance when compared to adding either hydrogenated Mg₃La or TiCl₃ alone. 4.3 wt% of H₂ can be released within 10 min at 400 °C in the LiBH₄ + Mg₃La + TiCl₃ system. The dehydrogenation activation energy of this system is 52.6 kJ mol⁻¹, which is much lower than that of pristine LiBH₄. In addition, the LiBH₄ + Mg₃La + TiCl₃ system preserves fast dehydrogenation kinetics and stable hydrogen storage capacity in the re-/dehydrogenation cycles.