This work combines materials development with hydrogen storage technology advancements to address onboard hydrogen storage challenges in light-duty vehicle applications. These systems are comprised of the vehicle requirements design space, balance of plant requirements, storage system components, and materials engineering culminating in the development of an Adsorbent System Design Tool that serves as a preprocessor to the storage system and vehicle-level models created within the Hydrogen Storage Engineering Center of Excellence. Computational and experimental efforts were integrated to evaluate, design, analyze, and scale potential hydrogen storage systems and their supporting components against the Department of Energy 2020 and Ultimate Technical Targets for Hydrogen Storage Systems for Light Duty Vehicles. Ultimately, the Adsorbent System Design Tool was created to assist material developers in assessing initial design parameters that would be required to estimate the performance of the hydrogen storage system once integrated with the full fuel cell system. Display omitted •Model analysis of adsorption-based hydrogen system for fuel cell applications.•Evaluation of various engineering design options for tank and balance-of-plant.•Thermodynamic equations to predict charging/discharging of activated carbon and MOF-5.•Prototype validation and model sensitivity analysis for data comparison.•Full-vehicle level analysis compared to DOE standards to determine applicability.