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Here we investigate the interactions of alkali and alkaline\u2010earth metal cations (Li\n                    <jats:sup>+<\/jats:sup>\n                    , Na\n                    <jats:sup>+<\/jats:sup>\n                    , K\n                    <jats:sup>+<\/jats:sup>\n                    , Be\n                    <jats:sup>2+<\/jats:sup>\n                    , Mg\n                    <jats:sup>2+<\/jats:sup>\n                    , Ca\n                    <jats:sup>2+<\/jats:sup>\n                    ) with five D\u2010symmetric PAHs\/nanographenes ranging from benzene to circumcircumcircumcoronene, aiming to elucidate the roles of aromaticity and topology in governing cation binding. We find that cation binding is strongest at the most aromatic peripheral six\u2010membered rings. Energy decomposition analysis reveals that binding is dominated by orbital interactions rather than electrostatics, with Be\n                    <jats:sup>2+<\/jats:sup>\n                    displaying anomalous, strongly covalent character and minimal ionic contribution. We introduce a novel ring\u2010based reactivity descriptor combining the Fukui function and electronic delocalization, which accurately predicts binding energies. In addition, a local topological indicator shows a strong correlation with cation\u2013PAH interactions and enables reliable predictions for graphene. Overall, our results demonstrate that aromaticity alone does not govern cation binding, but its interplay with local reactivity and topology is decisive, providing a unified framework that bridges chemical topology and computational chemistry.\n                  <\/jats:p>","DOI":"10.1002\/jcc.70337","type":"journal-article","created":{"date-parts":[[2026,4,13]],"date-time":"2026-04-13T11:00:59Z","timestamp":1776078059000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Does Aromaticity Drive Metal Cation Binding to Nanographenes? 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