The hydrogen storage of (TiZr0.1)xCr1.7-yFeyMn0.3 (1.05 < x < 1.2, 0.2 < y < 0.6) alloys, prepared by Ar plasma arc melting, were investigated by X-ray diffraction, pressure-composition- temperature (PCT). The results indicated that all (TiZr0.1)xCr1.7-yFeyMn0.3 (1.05 ≤x ≤ 1.2, 0.2 ≤y ≤ 0.6) alloys were determined as C14-type Laves phase, the cell parameters a, c and unit cell volume of (TiZr0.1)xCr1.1Fe0.6Mn0.3 (1.05 ≤x ≤ 1.2) alloys increased with increasing the (TiZr) super-stoichiometry from 1.05 to 1.2, and the value of a/c almost un-changed. The hydrogen absorption and desorption plateau pressure decreased from 5.6, 4.4-2.6, 2.2 MPa with the increase of (TiZr) super-stoichiometry from 1.05 to1.2 at 274 K respectively, and the hydrogen desorption plateau pressure decline was not obvious when the (TiZr) super-stoichiometry exceeded 1.15. The (TiZr0.1)1.1Cr1.1Fe0.6Mn0.3 alloy had the best comprehensive properties about the maximum and reversible hy-drogen storage capacity was 1.79 and 1.45 wt％ respectively. The cell parameters a, c and unit cell volume of (TiZr0.1)1.1Cr1.7-yFeyMn0.3(0.2 ≤y ≤ 0.6) alloys increased as the ratio of Fe/Cr content decreased. The hydro-genation and dehydrogenation plateau pressure decreased from 4.5, 3.4-1.0, 0.9 MPa respectively and the maximum hydrogen storage capacity increased from 1.79 to 2.0 wt％ as the Fe content reduced from 0.6 to 0.2 at 274 K. The maximum and the reversible hydrogen storage capacity were about 2.0 and 1.65 wt％ as the ratio of Fe/Cr was 0.13 (ie, (TiZr0.1)1.1Cr1.5Fe0.2Mn0.3 alloy), its relative molar enthalpy of dissociation hydrogen was 24.30 kJ/mol H2.