This paper presents a feasibility study of cryo-adsorption systems using low temperature adsorption materials for the on-board storage of hydrogen in a fuel cell vehicle. Charge and discharge validation experiments were performed using a 5 L semi-vehicle size tank. The tank was larger than the conventional lab scale test tank in order to clarify issues and evaluate the potential of this system for practical vehicle applications, and to provide targets for material development. Our results show that cryo-adsorption has a potential of higher hydrogen storage capacity in term of compactness and lightness than conventional high pressure tanks, provided that high volumetric density adsorption materials are available. Our results show that it is possible to obtain acceptable charge and discharge performance. They also show the necessity for further basic investigations into the heat transfer behavior during the charge and discharge of cold hydrogen into the system. In general, this concept is suitable for application in the context of a liquid hydrogen distribution infrastructure, which is widely used in industrial gas delivery today and is also expected to play an important role in hydrogen delivery systems for the transport sector.