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Here, we construct five phosphorescent molecular structural isomerization pairs based on both purely hydrocarbon and heteroatom\u2010containing aromatic compounds, elucidating how regioisomerization redistributes local aromatic character and skeletal rigidity, thereby selectively suppressing the dominant dissipative vibrational modes (C\u2550C and C\u2500N) in the triplet state. This selective vibrational restriction effectively reduces nonradiative decay loss and ultimately determines the efficiency and lifetime of triplet excitons. The representative regioisomeric phosphor further demonstrates long\u2010lived bioimaging capability with an extended in vivo imaging window, highlighting the practical relevance of this design strategy. This work identifies dominant vibrational coordinates as the primary origin of isomer\u2010dependent RTP behaviors and establishes a vibrationally resolved mechanistic framework for excited\u2010state relaxation engineering.<\/jats:p>","DOI":"10.1002\/anie.5600971","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T09:00:47Z","timestamp":1791450047000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mode\u2010Selective C\u2550C and C\u2500N Vibrational Coupling Modulates Nonradiative Decay in Regioisomeric Organic Phosphorescent Emission"],"prefix":"10.1002","author":[{"given":"Xiandong","family":"Chen","sequence":"first","affiliation":[{"name":"School of Chemistry and Materials Engineering Wenzhou University  Wenzhou P. R. 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