TiVMn and TiCrMn alloys are promising hydrogen storage materials for onboard application due to their high hydrogen absorption content. However, the traditional synthesis method of melting and continuous necessary heat treatment and activation process are energy- and time-consuming. There is rarely any report on kinetics improvement and nanoprocessing in TiVMn- and TiCrMn-based alloys. Here, through ball milling with carbon black as additive, we synthesized face-centered cubic (FCC) structure TiVMn- and TiCrMn-based nanoalloys with mean particle sizes of around a few to tens of mu m and with the crystallite size just 10 to 13 nm. Differential scanning calorimetry (DSC) measurements under hydrogen atmosphere of the two obtained TiVMn and TiCrMn nanoalloys show much enhancement on the hydrogen absorption performance. The mechanism of the property improvement and the difference in the two samples were discussed from microstructure and morphology aspects. The study here demonstrates a new potential methodology for development of next-generation hydrogen absorption materials.