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Herein, two covalently dimerized pyrene derivatives (1Py\u20102Py and 1Py\u20101Py) with distinct chemical linkages and crystal packing arrangements are presented. Remarkably, the radiative transition of pyrene is gradually unforbidden from 1Py\u20102Py to 1Py\u20101Py. Moreover, 1Py\u20102Py showcases 1D long\u2010range \u03c0\u2500\u03c0 stacking, while 1Py\u20101Py exhibits 2D herringbone packing formed by a vast network of intermolecular C\u2500H\u2219\u2219\u2219\u03c0 interactions. To the surprise, both high photoluminescence quantum yield (PLQY = 72.17%) and high hole mobility (<jats:italic>\u00b5<\/jats:italic> = 32.6 cm<jats:sup>2<\/jats:sup> V<jats:sup>\u22121<\/jats:sup> s<jats:sup>\u22121<\/jats:sup>) are simultaneously harvested in 1Py\u20101Py crystal, which are far superior to those in 1Py\u20102Py crystal (PLQY = 48.66% and <jats:italic>\u00b5<\/jats:italic> = 0.05 cm<jats:sup>2<\/jats:sup> V<jats:sup>\u22121<\/jats:sup> s<jats:sup>\u22121<\/jats:sup>). These findings underscore the potential of covalent pyrene dimer with 1\u2010position linkages as a promising organic semiconductor for the exceptional combination of strong luminescence and high mobility, which is substantially ascribed to the efficiently unforbidden emission and the favorable 2D charge transport pathways.<\/jats:p>","DOI":"10.1002\/adma.202419981","type":"journal-article","created":{"date-parts":[[2025,3,17]],"date-time":"2025-03-17T06:30:52Z","timestamp":1742193052000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":19,"title":["Integrating Strong Luminescence and High Mobility in Organic Single Crystals of Covalent Pyrene Dimers"],"prefix":"10.1002","volume":"37","author":[{"given":"Haichao","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University  Changchun 130012 P. R. 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