Our objective is to compare the volumetric storage capacity (VSC) and gravimetric storage capacity (GSC) on a systems basis for bulk hydrogenated Li3N (nominally LiNH2+2LiH) in its pure form (i.e., with no additives of any kind) and a nanoscale version comprised of hydrogenated Li3N encapsulated in a carbon host with 6-nm pores. We adopt the definitions of VSC and GSC used in the DOE targets, which are the net useful energy per total onboard storage system volume or mass, respectively. This definition excludes hydrogen remaining in the storage tank that is below the minimum pressure, flow, and temperature requirements of the fuel cell, as well as any hydrogen that must be combusted to heat the hydride bed to its required desorption temperature. It is important to emphasize that VSC is a property of the entire hydrogen storage system and is not an intrinsic material property. Consequently, VSC is applicable to any storage application but depends on the specific system design. Here, we elected to compare the bulk and nanoscale materials in the context of an LDV, which is important because developing materials that meet the DOE hydrogen storage system targets 2 has been (and continues to be) the focus of intense research efforts.