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In this work, the concept of adaptive co\u2010crystals featuring switchable host\u2010guest stoichiometry within the realm of pillararene\u2010based supramolecular chemistry is proposed. This strategy allows for the rational design of a diverse range of through\u2010space charge\u2010transfer co\u2010crystals, enabling dynamic modulation of photoluminescence in the solid state. Experimental and theoretical findings unveil two distinct phases within each set of co\u2010crystal architectures, characterized by different donor\/acceptor stoichiometric ratios as well as molecular packing modes. Notably, these co\u2010crystalline phases undergo vapor\u2010induced stoichiometry switching and structural interconversion, resulting in unique charge\u2010transfer transition states and enabling reversible control over photoluminescent behavior. Particularly, this dynamic modulation of the cavity apertures, driven by stoichiometric variation, facilitates highly selective capture and release of 1\u2010bromoalkane under mild conditions. The present study highlights the potential application of vapor\u2010mediated co\u2010crystals with switchable stoichiometry as a supramolecular strategy for modulating the intrinsic characteristics of intermolecular donor\u2013acceptor materials.<\/jats:p>","DOI":"10.1002\/adma.202514110","type":"journal-article","created":{"date-parts":[[2025,11,17]],"date-time":"2025-11-17T07:03:48Z","timestamp":1763363028000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Adaptive Co\u2010Crystals with Switchable Host\u2010Guest Stoichiometry for Dynamic Regulation of Photoluminescence"],"prefix":"10.1002","volume":"38","author":[{"given":"Minzan","family":"Zuo","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials Jiangxi Normal University  Nanchang 330022 P. R. 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