The phase structures and hydrogen absorption-desorption properties of Ti-V-Cr-Mn alloys were investigated. It is found that the increasing V content is effective for enhancing the hydrogen absorption capacity and flattening the hydrogen desorption plateau, while it depresses the hydrogen desorption plateau pressure.With the increase of V content, two phases of BCC and C14 Laves of the alloys transform into a single BCC phase. The maximum and effective hydrogen storage capacities among studied alloys are 3.98 and 2.51 wt.%, respectively, which open the hope to bring Ti-V-based alloy into the reach of practical application for onboard hydrogen storage systems in fuel cell powered vehicles.