In this study, influence of Al substitution on hydrogen storage properties of Ti₂CrV alloy has been investigated in detail. The alloys Ti_2–xCrVAl_x (x = 0.05, 0.1) were synthesized by arc melting method, and composition, type of crystal structure and hydrogen storage properties were evaluated. X-ray diffraction studies confirmed that all the alloys form single-phase bcc structures. Ti_1.95CrVAl_0.05 alloy is found to absorb a maximum of 3.9 wt% of hydrogen at room temperature and moderate hydrogen pressure. The plateau pressure of the studied alloys increases with an increase in Al concentration. The results confirm that among the studied alloys, Ti_1.95CrVAl_0.05 alloy shows the fastest hydrogen absorption kinetics and improved cyclic stability with a marginal decrease in total hydrogen absorption capacity compared to the parent alloy.