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Existing crystalline photoactivated RTP systems generally require pretreatment and have not enabled RTP\/TADF regulation. Here, we demonstrate for the first time that intrinsic photoactivated RTP can be achieved in a pretreatment\u2010free crystalline system, while the occurrence of TADF can be switched on or off through rational host\u2010guest engineering. Dinaphtho[2,1\u2010b:1\u2032,2\u2032\u2010d]furan (OA) exhibits intrinsic photoactivated RTP at 77\u00a0K, when incorporated into three crystalline hosts, forms a general crystalline photoactivated platform at room temperature. Experimental and calculational results indicate that energy level matching and exciton lifetime govern RTP\/TADF modulation. Specifically, long\u2010lived excitons in host dibenzofuran (DBF) enable simultaneous RTP and TADF through host\u2010guest energy transfer, whereas methyl 4\u2010(methylamino)benzoate (MAB) and boric acid (BA) as hosts suppress TADF due to mismatched energy levels or rapid exciton quenching. Nevertheless, their RTP emission is facilitated by high crystallinity and rigid hydrogen\u2010bonding networks. Mechanistic analysis indicates that UV irradiation regulates excited\u2010state carrier concentration and transition probability, thereby enabling photoactivation. This work establishes a design strategy for crystalline photoactivated luminescent materials with potential applications for time\u2010dependent anti\u2010counterfeiting.<\/jats:p>","DOI":"10.1002\/advs.77468","type":"journal-article","created":{"date-parts":[[2026,8,29]],"date-time":"2026-08-29T10:56:03Z","timestamp":1788000963000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Photoactivation\u2010Enabled Tunable Room\u2010Temperature Phosphorescence and Thermally Activated Delayed Fluorescence in Crystalline Materials"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-6163-7702","authenticated-orcid":false,"given":"Lisha","family":"Zhang","sequence":"first","affiliation":[{"name":"Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Frontiers Science Center for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai China"},{"name":"Laboratory of Organic Electronics Department of Science and Technology Link\u00f6ping University  Norrk\u00f6ping Sweden"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongping","family":"Wu","sequence":"additional","affiliation":[{"name":"Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center Frontiers Science Center for Materiobiology and Dynamic Chemistry School of Chemistry and Molecular Engineering East China University of Science and Technology  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ihor","family":"Sahalianov","sequence":"additional","affiliation":[{"name":"Laboratory of Organic Electronics Department of Science and Technology Link\u00f6ping University  Norrk\u00f6ping 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