In this study, we evaluated the effects of a mechanical treatment by cold rolling (CR) and ball milling (BM) on the first hydrogenation of Ti1V0.9Cr1.1 alloy. The as-cast alloy has a body-centered cubic (BCC) crystal structure, and the first hydrogenation at room temperature under 20 bars of hydrogen is practically impossible. However, the samples mechanically activated by CR or BM readily absorbed hydrogen. The sample cold-rolled for one pass exhibited faster kinetics than the sample ball-milled for five minutes, but both samples reached the same storage capacity of 3.6 wt % hydrogen. Increasing the amount of rolling or the milling time decreased the hydrogen capacity. CR is considered the best and most efficient method for the activation of Ti1V0.9Cr1.1 alloy.