The microstructure and hydrogen absorption and desorption properties of (VFe)48Ti26Cr26-xMox (0≤x≤5) alloys were investigated. XRD and PCT testing results show that both the lattice constants and plateau pressure increase with the rising of Mo content, and the hydrogen absorption/desorption capacities have no significant change when 0≤x≤2. While the effective desorption capacities maintain more than 2%. When x=1, the alloy shows the maximum hydrogen absorption capacity of 3.59% and the maximum desorption capacity of 2.08%, with a plateau pressure of 0.337 MPa at room temperature. SEM and EDS analyses show that all of the alloys consist of bcc main phase, Laves phase and rare earth oxide phase. Mo mainly distribute in the bcc main phase, and a small amount of Mo exist in the Laves phase.