Here we report a Ti V -10 wt.% C alloy with a unique lattice and microstructure for hydrogen storage development. Different from a traditionally synthesized Ti V alloy prepared by a melting method and having a body-centered cubic (BCC) structure, this Ti V -C alloy synthesized by a mechanical alloying method is with a face-centered cubic (FCC) structure (space group: Fm-3m No. 225). The crystalline size is 60 nm. This alloy may directly absorb hydrogen near room temperature without any activation process. Mechanisms of the good kinetics from lattice and microstructure aspects were discussed. Findings reported here may indicate a new possibility in the development of future hydrogen storage materials.