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This study emphasizes the catalytic function of TiF3on hydrogen storage properties and the reaction mechanism of the MgH2-Na3AlH6-LiBH4produced by employing the ball-milling technique, which has a molar ratio of 1:1:4. It discovered that the mixture of Na3AlH6and LiBH4reacted through a metathesis reaction and transformed into Li3AlH6and NaBH4composite upon the ball milling procedure. MgH2-Li3AlH6-NaBH4destabilized system with TiF3catalyst has displayed four decomposition tiers throughout the heating procedure. The initial tier of hydrogen release in the composite occurs at temperatures of 100 °C and 75 °C lower than in the catalyst-free composite. Continuous heating resulted in two through four dehydrogenation tiers, with an overall capacity of 10.1 wt% hydrogens released (at temperatures of 200 °C, 350 °C, and 400 °C, respectively). In contrast to the Mg-Na-Al-Li-B-H catalyst-free composite, incorporating the TiF3catalyst demonstrates a faster hydrogen uptake and release rate. The apparent activation energy (Ea) for the dissociation of Li3AlH6, MgH2, and NaBH4in the composite with TiF3catalyst was remarkably abridged compared to the catalyst-free ternary system (Kissinger plot; 23, 20, and 13 kJ/mol, respectively for doped composite). TiF3's considerable catalytic performance is ascribed to the in-situ production of AlTi and AlF phases during the dehydrogenation process of TiF3and Li3AlH6. Once generated, the AlTi and AlF phase serves as a genuine catalyst in the MgH2-Na3AlH6-4LiBH4-TiF3ternary system.