Hydrogenation properties of the vanadium-rich ternary V-Ti-Cr alloy was investigated, which is of interest as a hydrogen carrier for fuelcell vehicles. The dependence of hydrogen content of the hydrides with low plateau pressure ( phase) on the unit cell volume of the dehydrogenated alloys ( phase) is found to be different from that of the hydrides ( phase) with high plateau pressure. By optimizing the alloy composition, a large effective hydrogen storage capacity of 2.62 mass% is obtained.