• Co-modification with Ce doping and cold rolling enables room-temperature activation of V70Ti10Cr20 alloy without incubation, achieving 4 wt% hydrogen capacity within 12 minutes.
• CeO2 particles act as active sites that facilitate hydrogen penetration through the surface oxide layer, while cold rolling introduces dislocations that create rapid diffusion pathways.
• The synergistic effect of Ce alloying and cold rolling significantly outperforms either method alone, reducing activation temperature and time dramatically.
• This work provides a practical engineering strategy for improving the activation performance of vanadium-based hydrogen storage alloys, advancing their industrial application.