A nanoconfined version, (LiNH2+2LiH)@(6-nm PC), was also synthesized by infiltrating a porous carbon (PC) with 6-nm pores using a procedure we developed previously. Our prior work showed that the intermediate imide Li2NH could be avoided for the nanoconfined material, allowing full dehydrogenation from (LiNH2+2LiH)@(6-nm PC), Unexpectedly, we find that the modeled systems-level usable hydrogen capacity (per unit volume or mass of the storage system) of the nanoscale material is greater than that of the bulk, even though the bulk material has a much higher capacity on a materialsbasis (per unit volume of material). This showed that a co-design approach, in which materials synthesis, characterization, and systems modeling inform each other to arrive at an optimal material-based storage system, is essential to determine the best material for a specific application. A second important conclusion is that a host for hydride nanoparticles can be designed to achieve properties superior to the bulk material without sacrificing capacity, i.e. without incurring "dead weight" as previously assumed. This result also shows that relying on the intrinsic properties of a storage material to assess its performance without consideration of the complete storage system design and its dynamic operation can lead to erroneous conclusions. Finally, our results demonstrate that a nanoporous host can be a multifunctional material, simultaneously modulating the thermodynamics, kinetics, and heat transfer properties of a metal hydride, thereby transforming the hydride from an unusable material to one with potential to perform hydrogen storage for a particular use case.