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In this study, we rationally designed a series of benzimidazole\u2010based donor\u2013\u03c0\u2013acceptor (D\u2013\u03c0\u2013A) compounds using triphenylamine (TPA) as the donor and benzimidazole as the acceptor, functionalized with flexible alkyl chains to modulate intermolecular packing. Benefitting from their rigid planar molecular conformation, all four compounds exhibit intense blue fluorescence in both solution and the PMMA\u2010doped state. Among them, the highest luminescence efficiencies of the molecule <jats:bold>C0<\/jats:bold> in the DCM\u2010 and PMMA\u2010doped films reach 78.72% and 65.28%, respectively. Notably, their PMMA\u2010doped films also exhibit obvious yellowish\u2013green afterglows after\u00a05\u00a0s continuous UV irradiation. In the solid state, the chain\u2010free molecule <jats:bold>C0<\/jats:bold> forms a staggered stacking with intermolecular hydrogen bonds, resulting in a bright excimer emission. As the alkyl chain length increases, the added steric bulk gradually suppresses the intermolecular interactions, inducing a significant transition from excimer emission to blue\u2010shifted monomer emission. Furthermore, the nitrogen atom of benzimidazole endows these luminophores with pronounced acid\u2010responsive fluorescence behavior. By exploiting the distinct luminescent contrast between the excimer and monomer emissions of <jats:bold>C0<\/jats:bold>, we developed a temperature\u2010responsive fluorescence system through embedding <jats:bold>C0<\/jats:bold> into a phase\u2010change matrix, which enables a reversible thermochromic fluorescence switching. This work provides a valuable strategy for designing dual\u2010state emission and stimuli\u2010responsive benzimidazole\u2010based materials with potential applications in optical sensing and display technologies.<\/jats:p>","DOI":"10.1002\/asia.202500600","type":"journal-article","created":{"date-parts":[[2025,8,13]],"date-time":"2025-08-13T19:09:19Z","timestamp":1755112159000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Benzimidazole\u2010Based Dual\u2010State Luminophores with Acid Responsiveness and Thermo\u2010Switchable Emission in Phase\u2011Change Matrix"],"prefix":"10.1002","volume":"20","author":[{"given":"Xueru","family":"Shan","sequence":"first","affiliation":[{"name":"State Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Lab of Science and Technology of Eco\u2010Textile Ministry of Education College of Chemistry and Chemical Engineering Donghua University  Shanghai 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