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Herein, we report a synthetic approach to NIR\u2010responsive materials by self\u2010assembly of hydrogen\u2010bonded organic frameworks (\n                    <jats:bold>HOF\u20101\/2\/3<\/jats:bold>\n                    ) from multifunctionalized Ru\u2010components incorporating chiral, photoactive, H\u2010bonding, \u03c0\u2010stacking, and protonation\/deprotonation subunits. Significantly, protonation of the imidazole\u2010subunits in\n                    <jats:bold>HOF\u20103<\/jats:bold>\n                    promotes densified packing to extend NIR absorption tail up to 1100\u00a0nm with a narrowed bandgap of 1.41\u00a0eV, meanwhile leads to spontaneous resolution of enantiomeric\n                    <jats:bold>\u0394\u2010\/\u039b\u2010HOF\u20103<\/jats:bold>\n                    . Consequently, remarkably enhanced photothermal effect and photocatalytic performance, including chiroptical activity induced by circularly polarized NIR light, are achieved through synergy of direct one\u2010 and multi\u2010photon NIR absorption, underscoring effectiveness to bring multifunctionalities into ordered HOFs for generation of robust and effective materials with multimode NIR responsiveness.\n                  <\/jats:p>","DOI":"10.1002\/anie.202511088","type":"journal-article","created":{"date-parts":[[2025,6,17]],"date-time":"2025-06-17T05:05:34Z","timestamp":1750136734000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Merging One\u2010 and Multi\u2010Photon Processes in Hydrogen\u2010Bonded Organic Frameworks for Enhanced NIR Light\u2010Driven Photothermal and Photochemical 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