One of the most important technologies for the sustainable development of energy in the future is solid-state hydrogen storage. This study employed etching methods to fabricate two-dimensional layered catalyst Mo2Ti2C3 MXene, which was compared with unetched MAX phases Mo2Ti2AlC3 and Ti3C2, as well as Mo2C. Through mechanical ball milling, these materials were mixed with MgH2 to prepare composite materials, including MgH2 + Ti2C3, MgH2 + Mo2C, MgH2 + Mo2Ti2AlC3, and MgH2 + Mo2Ti2C3. According to the study, Mo2Ti2C3 demonstrates the synergistic catalytic actions of Ti and Mo in contrast to Ti2C3 and Mo2C. The composite material MgH2 + Mo2Ti2C3 lowers the initial dehydrogenation temperature of MgH2 to 180 °C, which is 165 °C lower than pure MgH2. After 30 min at 250 °C, the dehydrogenation amount is approximately 5.85 wt%. Hydrogen absorption begins at 40 °C and reaches approximately 5.75 wt% at 150 °C. Additionally, it maintains a reversible hydrogen storage capacity of up to 96 % even after 20th cycles at 300 °C. This is because Mo2Ti2C3 has one less layer of Al than Mo2Ti2AlC3, which results in a wider interlayer spacing, more active sites for MgH2, and facilitates hydrogen molecule dissociation and recombination.