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Alternatively, recently discovered small molecules to enhance the Raman signal intensities through their self\u2010stacking, termed stacking\u2010induced intermolecular charge transfer\u2010enhanced Raman scattering (SICTERS), offer ultrasensitive in vivo Raman imaging free of substrates. Molecular engineering to increase the SICTERS intensity and to tune photothermal conversion efficiency of these molecules is critical for furthering their biomedical application but not yet feasible. Here, by increasing the length of side chain and introducing the benzene ring to bis\u2010thienyl\u2010substituted benzobisthiadiazole, this study demonstrates an optimized molecule BBTPPRO that possesses both high SICTERS intensity and photothermal conversion efficiency (31.19%). The prepared BBTPPRO nanoparticles achieve intraoperative Raman image\u2010guided photothermal therapy (PTT) of orthotopic mouse colon tumor. 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