This study successfully synthesized lamellar Zn2Ti3O8, TiO2, and rod-shaped ZnO catalysts through hydrothermal and calcination methods, comparing the catalytic performance of the three catalysts on MgH2. Notably, Zn2Ti3O8 demonstrated significant synergistic enhancement in the dehydrogenation temperature and desorption kinetics of MgH2. Experimental results revealed that the MgH2 + 12 wt% Zn2Ti3O8 composite material commenced dehydrogenation at approximately 185 °C, around 160 °C lower than pure MgH2. Furthermore, at 325 °C, MgH2 release d only 3.06 wt% H2 within 20 min, whereas the Zn2Ti3O8 doped composite system achieved the same hydrogen release at 225 °C within 7 min. After complete dehydrogenation, the MgH2 + 12 wt% Zn2Ti3O8 composite material-initiated hydrogen absorption at 40 °C and absorbed approximately 6.05 wt% H2 within 60 min at 200 °C. The activation energies for hydrogen absorption and desorption of the composite material decreased by 22.25 kJ·mol-1 and 44.67 kJ·mol-1, respectively, compared to pure MgH2. Cycling experiments demonstrated that after 20 cycles, the MgH2 + 12wt% Zn2Ti3O8 composite material maintained excellent cyclic stability, with hydrogen storage capacity still exceeding 95%. Hence, this composite material exhibits outstanding catalytic and hydrogen storage performance, holding potential application value in enhancing hydrogen release rates and reducing activation energy.