AB2-type Ti-based hydrogen storage alloys are considered promising candidates for the hydrogen feeding system in hydrogen-metallurgy application. In this work, Ti0·87Zr0.15MnxCr1.75-xV0.25 (x = 1.25–1.5), Ti0·87Zr0·15Mn1·5Cr0.5-y(VFe)y (y = 0.25–0.43) and Ti0.85+zZr0.15Mn1·5Cr0·07(VFe)0.43 (z = 0–0.05) alloys were synthesized using induction levitation melting, where ferrovanadium VFe consists of 80 wt% V and 20 wt% Fe. Subsequently, their microstructures and hydrogen storage performances were systematically investigated. The results demonstrate that all alloy samples exhibit a single C14 Laves phase structure with uniform element distribution. With the increment of Cr/Mn, VFe/Cr ratio, or Ti stoichiometry, the alloys exhibit enhanced hydrogen storage capacity, accompanied by a decrease in hydrogenation equilibrium pressure because of interstitial volume expansion or hydrogen affinity improvement, which is also supported by density functional theory calculations. Considering the application of hydrogen metallurgy, Ti0·86Zr0·15Mn1·5Cr0·07(VFe)0.43 alloy is regarded as a promising candidate, exhibiting a saturated capacity of 2.01 wt% H2, an effective reversible capacity of 1.91 wt% H2, rapid hydrogenation kinetics, excellent cyclic durability and low costs. This work provides valuable insights into the compositional design of hydrogen storage alloys for the hydrogen feeding system in hydrogen metallurgy applications.