The structure and properties of V55Ti20.5Cr18.1Fe6.4 alloys were studied. It is found that with increasing Ni content, the effective hydrogen capacity increases first, and then decreases, and the hydrogen desorption pressure increases and the hydrogen absorption kinetic properties are improved first, and then decayed. The hydrogen absorption and desorption properties of V55Ti20.5Cr18.1Fe6.4 can be improved by substitution of 0.1at%Ni. The change of cell volume, the increase of hydrogen desorption pressure and the appearance of impurity phases are the main reasons influencing the hydrogen absorption and desorption properties by substitution of Ni for V for the alloy.