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Here, a diketopyrrolopyrrole\u2010derived photosensitizer (DTPA\u2010S) is developed via thionation of carbonyl groups within the diketopyrrolopyrrole skeleton, which results in a large bathochromic shift of 81 nm, endowing the photosensitizer with strong NIR absorption at 712 nm. DTPA\u2010S is then introduced with a functional biomolecule (N<jats:sub>3<\/jats:sub>\u2010PEG<jats:sub>2000<\/jats:sub>\u2010RGD) via click reaction for the construction of integrin \u03b1v\u03b23 receptor\u2010targeted nano\u2010micelles (NanoDTPA\u2010S\/RGD), which endows the photosensitizer with a further superlarge absorption redshift of 138 nm, thus extending the absorption maxima to \u2248850 nm. Remarkably, thiocarbonyl substitution increases the nonbonding characters in frontier molecular orbitals, which can effectively suppress the nonradiative vibrational relaxation process via reducing the reorganization energy, enabling efficient reactive oxygen species (ROS) generation under 880 nm excitation. Screened by in vitro and in vivo assays, NanoDTPA\u2010S\/RGD with high water solubility, excellent tumor\u2010targeting ability, and photodynamic\/photothermal therapy synergistic effect exhibits satisfactory phototherapeutic performance. Overall, this study demonstrates a new design of efficient NIR\u2010triggered diketopyrrolopyrrole photosensitizer with facile installation of functional biomolecules for potential clinical applications.<\/jats:p>","DOI":"10.1002\/advs.202407727","type":"journal-article","created":{"date-parts":[[2024,10,16]],"date-time":"2024-10-16T16:38:17Z","timestamp":1729096697000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Molecular Engineering of a Tumor\u2010Targeting Thione\u2010Derived Diketopyrrolopyrrole Photosensitizer to Attain NIR Excitation Over 850 nm for Efficient Dual Phototherapy"],"prefix":"10.1002","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4974-9496","authenticated-orcid":false,"given":"Gang","family":"Xu","sequence":"first","affiliation":[{"name":"Jiangsu Province Hi\u2010Tech Key Laboratory for Biomedical Research School of Chemistry and Chemical Engineering Southeast University  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