The hydrogen storage capacities and crystal structure of AB(2)-type Ti-Mn based alloys Ti0.8Zr0.2Mn2-xCrx(x = 0.2, 0.4, 0.6, 0.8, 1.0), Ti0.8Zr0.2Mn1.8V0.2 and Ti0.9ZrxMn1.8-yCryV0.2(x=0.1, 0.15,0. 2; y = 0.2, 0.4) have been studied. The results show that the substitution of Zr for Ti of the side A and stoichiomentric excess of the side A are effective on improving the activation and increasing the absorption-desorption hydrogen capacity. The hydrogen storage capacity increases monotonously with increasing the lattice parameters and unit cell volume. The hydrogen storage capacity of Ti-Mn based alloys can reach 235 ml/g for a greater than or equal to0.489 4 nm, c greater than or equal to0.804 0 nm, or V greater than or equal to0.166 8 nm(3).