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Summary In this work, we designed and addressed the hydrogen storage capacities of Li and Sc doped novel C8N8 cages using dispersion corrected density functional theory (DFT‐D3). The stabilities of C8N8Li2 and C8N8Sc2 cages were confirmed by chemical hardness, HOMO‐LUMO gaps, and molecular dynamic simulations. Both C8N8Li2 and C8N8Sc2 could adsorb 5H2 molecules with an average hydrogen adsorption energy of 0.187 and 0.291 eV/H2, keeping the original structure intact. The H2 molecules interacted with the Li/Sc via Niu‐Rao‐Jena and Kubas type interactions, and the charge re‐distribution in H2 molecules in C8N8Li2‐nH2 and C8N8Sc2‐nH2 showed that H2 molecules were adsorbed in a quasi‐molecular fashion. The molecular dynamics simulation revealed the thermal stability and structural integrity of Li and Sc decorated C8N8 cages at a relatively high temperature of 400 K, and at 300 K most of the H2 molecules were desorbed from the host material, keeping their initial structure intact, which confirmed their reversibility. The practical H2 storage capacities of C8N8Li2 and C8N8Sc2 cages at temperature and pressure ranges of 40 to 160 K, 40 to 180 K, and 10 to 60 bar were found to be 8.32 wt%, and 6.33 wt%, which were fairly above the target of US‐DOE (5.5 wt% by 2025). At the temperature and pressure range of 220 to 280 K and 30 to 60 bar, the gravimetric density of both the cages was approximately 5.5 wt%. Hence, the newly designed C8N8Li2 and C8N8Sc2 cages can be considered as potential candidates for reversible hydrogen storage systems.