The aim of the present study is the development of a multiscale modeling and optimization framework for hydrogen storage in carbon-based nanoporous adsorbents. The outlined methodology is generic and can be easily adapted to the storage of several gases of relevant importance and/or different physisorbing nanoporous materials. The results indicate clearly how operating constraints (such as temperature limitations arising from safety considerations) can affect the material design in terms of its pore size distribution and how material design constraints (such as those arising from manufacturing limitations) can effect the operation and efficiency of the process. The ultimate objective is to systematically reveal the strong and highly related synergistic benefits between process design/operation decisions and material design aspects so as to ensure an economically attractive, technically feasible, and safe process. (c) 2006 American Institute of Chemical Engineers.