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For the first time, this study introduces a novel modular \u201cOff\u2010Brighter\u201d persistent luminescence (PersL) theranostic strategy for visualized cancer therapy. The nano\u2010agent integrates two functional modules: a proton\u2010responsive PersL imaging brick (ZR) optimized via dye\u2010sensitization, and a GSH\u2010responsive synergistic photothermal\/chemodynamic therapy brick (PAHIR\u2010Fcss) loaded with IR808 and FcSH. FcSH temporarily quenches ZR's PersL, creating \u201cGSH\u2010proton\u201d tandem\u2010responsive \u201cOff\u2010Brighter\u201d activation that enhances luminescence 12.3\u2010fold and achieves tumor imaging contrast of 274.95. Real\u2010time imaging guided drug delivery monitoring, identifying the 3rd h post\u2010injection as optimal for combination therapy. The synergistic photothermal\/chemodynamic approach attained 96.2% tumor suppression in murine breast cancer models. Subsequent PersL imaging\u2010based assessment determined that a single 14\u2010day treatment course optimizes efficacy while preventing overtreatment risks. The modular design enables free exchange of imaging and therapeutic components, offering a versatile, generalizable platform for tailored clinical applications.<\/jats:p>","DOI":"10.1002\/smll.74772","type":"journal-article","created":{"date-parts":[[2026,7,23]],"date-time":"2026-07-23T09:44:01Z","timestamp":1784799841000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Modularized GSH\u2010Proton Tandem\u2010Responsive \u201cOff\u2010Brighter\u201d Persistent Luminescent Nano\u2010System for Visualized Synergetic PTT &amp; CDT of Mastocarcinoma"],"prefix":"10.1002","volume":"22","author":[{"given":"Chang","family":"Yin","sequence":"first","affiliation":[{"name":"Key Laboratory of Functional Polymer Materials of the Ministry of Education Institute of Polymer Chemistry College of Chemistry Nankai University  Tianjin 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