The alloys which compositions were represented by the formula, $Ti_{(0.22+X)}Cr_{(0.28+1.5X)}V_{(0.5-2.5X)}$ ($0{leq}X{leq}0.12$), had the total hydrogen storage capacity higher than 3 wt% and the effective hydrogen storage capacity higher than 1.4 wt%. Particularly, among all the tested alloys, the $Ti_{0.32}Cr_{0.43}V_{0.25}$ alloy exhibited the best effective hydrogen storage capacity of 1.65 wt%. Furthermore, the reversible bcc${leftrightarrow}$fcc structural transition was observed with hydrogenation and dehydrogenation, which predicted the possibility of pressure cycling. EDS analysis revealed micro-segregation, which suggested the necessity of microstructure homogenization by heat treatment. The $Ti_{0.32}Cr_{0.43}V_{0.25}$ alloy was selected for heat treatment and for other related studies. The results showed that the total and the effective hydrogen storage capacity increased to 3.7 wt% and 2.3 wt%, respectively. The flatness of the plateau region was also greatly improved and heat of hydride formation was determined to be approximately -36 kJ/mol $H_2$.