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Here, a new crystal engineering strategy is introduced in which host matrices are rationally designed to accommodate a predefined class of dopants and promote favorable host\u2013guest interactions. This tailored\u2010dopant matrix concept is demonstrated for dopant\u2010induced organic room\u2010temperature phosphorescence (RTP) using carbazole\u2010based matrices and benzoindole\u2010based dopants, a prototypical RTP system. Guided by the hypothesis that a herringbone packing of carbazole units promotes synergistic structural interactions with the dopant, a multiscale theoretical methodology is first developed to elucidate the intermolecular interactions stabilizing this motif in pristine carbazole\u2010based crystals. These insights enable the design and synthesis of new host architectures exhibiting the targeted packing arrangement. Ultimately, the resulting single\u2010crystalline host\u2013guest materials exhibit long\u2010lived organic RTP, with phosphorescence lifetimes of several hundred milliseconds. This work could establish dopant\u2010tailored crystal engineering as a potential new paradigm for designing functional doped organic semiconductor crystals with tailored optoelectronic properties.<\/jats:p>","DOI":"10.1002\/anie.8252460","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T16:56:32Z","timestamp":1786553792000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dopant\u2010Tailored Matrices: A Crystal Engineering Strategy for Organic Room\u2010Temperature Phosphorescent Host\u2013Guest Systems and Beyond"],"prefix":"10.1002","volume":"65","author":[{"given":"Catherine","family":"Demangeat","sequence":"first","affiliation":[{"name":"Building Blocks for FUture Electronics Laboratory IRL 2002 CNRS\u2010Sorbonne Universit\u00e9\u2010Yonsei University Yonsei University  Seoul Republic of Korea"},{"name":"Department of Engineering Science The University of Electro\u2010Communications  Tokyo Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Raphael","family":"Rullan","sequence":"additional","affiliation":[{"name":"ENS de Lyon CNRS Lyon France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yipeng","family":"Tang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices South China University of Technology  Guangzhou P. 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