The physical upper limit of hydrogen uptake for powder and compressed pellet MIL-101 has been experimentally investigated. Maximum uptake in pellets at 20 K achieves 9.6 wt% and 42 g L-1. Moreover, cryo-adsorption of hydrogen on pellets compared to liquid H-2 possesses a larger temperature window for operation without boil-off loss, which will be beneficial for industrial applications.