The microstructure and hydrogen storage properties of low V content(Ti0.46Cr0.54) 100-x V x(x = 2.5–7.1, at%) and(TiyCr1-y)95V5(y = 0.38–0.54) alloys were investigated. These alloys were prepared by arc melting and copper mould suction casting. The structures of as-cast(Ti0.46Cr0.54) 100-x V x(x = 2.5, 5.0, and 7.1) alloy ingots evolve with V contents from pure Laves-(x = 2.5) to dual-phase TiCr2-BCC structures(5.0 and 7.1), whereas the suction-cast(Ti0.46Cr0.54) 100-x V x(x = 2.5, 5.0, and 7.1) alloys only contain single BCC phase. The suctioncast alloy rod(Ti0.46Cr0.54)95V5, containing only 5.0 at% V is shown to possess the optimum hydrogen absorption capacity, with the maximum hydrogen content of 3.14 wt%. Furthermore, the hydrogen storage properties of the suction-cast low V alloys(TiyCr1-y)95V5(y = 0.38–0.54) are sensitive to Ti/Cr ratios and only those alloys with Ti/Cr ratios close to the CN14 cluster [Ti7Cr8 ] have good hydrogen storage properties. The microstructure and hydrogen storage properties of low V content (Ti0.46Cr0.54) 100-x V x (x = 2.5-7.1, at%) and (TiyCr1-y) 95V5 (y = 0.38-0.54) alloys were investigated. These structures were prepared by arc melting and copper mold suction casting. The structures of as-cast (Ti0.46Cr0.54) 100-x V x (x = 2.5, 5.0, and 7.1) alloy ingots evolve with V contents from pure Laves - (x = 2.5) to dual-phase TiCr2-BCC structures (5.0 and 7.1), while the suction-cast (Ti0.46Cr0.54) 100-x V x (x = 2.5, 5.0, and 7.1) alloys only contain single BCC phase. The suction cast alloy rod (Ti0.46Cr0.54) 95V5 containing only 5.0 at% V is shown to have the optimum hydrogen absorption capacity, with the maximum hydrogen content of 3.14 wt%. the suction-cast low V alloys (TiyCr1-y) 95V5 (y = 0.38-0.54) are sensitive to Ti / Cr ratios and only those alloys with Ti / Cr ratios close to the CN14 cluster [Ti7Cr8]