The hydrogen storage properties of V-Ti-Cr-Fe alloys with compositions of V(30 at%)-Ti(15 at%~55 at%)-Cr(7 at%~43 at%)- Fe(2 at%~18 at%) were studied in this paper. It is found that the hydrogen absorption capacities and the effective hydrogen capacities of the alloys are largely dependent on the Ti/(Cr+Fe) ratio. The alloy shows the largest effective hydrogen capacity at a Ti/(Cr+Fe) ratio of 1.0. With the increase of Ti/(Cr+Fe) ratio (0.9~1.05), the lattice parameters of the alloys and the enthalpy of hydrides grow, and the hydrogen desorbing plateau pressure declines. The alloy of V30Ti35Cr25Fe10 with 10at% Fe exhibits a hydrogen capacity of 3.6wt% and an effective hydrogen capacity of 2.0wt% at 298 K.