Presence of curvature is considered as a tuning parameter to activate the hydrogen storage capability of carbon nanostructures. Here, we explicate the role of ‘intra-curvature’ in a set of single-walled carbon nanohorns (SWCNHs), to adsorb light metal ad-atoms (M) e.g. Li, Na, Ca and subsequently explore the metal-doped systems for hydrogen storage application using density functional theory. The binding strength of ad-atoms on SWCNHs of different curvature is correlated with the π  electron occupancy of the corresponding carbon ring. Higher π  electron occupancy causes significantly high binding energy of the metal ad-atoms (M), thereby indicating high stability of those M−C bonds for intracurvature values more than 11⁰, even at a higher temperature. After full hydrogenation, Li-doped SWCNHs are found to contain a maximum of 7.5 wt % of hydrogen. Overall, our results indicate that Li-doped SWCNHs with intra-curvature values higher than 11⁰, is a potential candidate for hydrogen storage.