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Herein, we report a photoactivatable molecular magnetic resonance\/fluorescence (MR\/FL) imaging probe for sensitive HCC imaging and potent tumor eradication that exploits the intrinsically RNA\u2010enriched nature of HCC. Upon light irradiation, singlet oxygen (\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    ) triggers in situ furan\u2013RNA crosslinking, prolonging its rotational correlation time (\n                    <jats:italic>\u03c4<\/jats:italic>\n                    <jats:sub>r<\/jats:sub>\n                    ), thereby markedly amplifying\n                    <jats:italic>r<\/jats:italic>\n                    <jats:sub>1<\/jats:sub>\n                    relaxivity. Notably, this light\u2010activated furan\u2013RNA crosslinking strategy affords a 75% enhancement in tumor MR signal, significantly outperforming clinically used MR contrast agents. FL imaging further reveals prolonged tumor retention with detectable signals persisting for over 14 days, highlighting its potential for longitudinal monitoring of therapeutic response. Concurrently, photo\u2010generated\n                    <jats:sup>1<\/jats:sup>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    and following RNA crosslinking results in multiple cell death mechanism, including pyroptosis, ferroptosis and RNA interference, enabling sustained tumor suppression. This work presents the first photoactivatable RNA\u2010targeted MR\/FL imaging probe and establishes a new paradigm that integrates molecular\u2010level MRI signal amplification, long\u2010term tumor retention, and multi\u2010pathway synergistic antitumor therapy for holistic HCC management.\n                  <\/jats:p>","DOI":"10.1002\/anie.8894678","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T10:30:31Z","timestamp":1786357831000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Photo\u2010Generated\n                    <sup>1<\/sup>\n                    O\n                    <sub>2<\/sub>\n                    Triggers In Situ RNA Crosslinking for High\u2010Contrast Tumor MRI and Effective Tumor Suppression"],"prefix":"10.1002","volume":"65","author":[{"given":"Ying","family":"Luo","sequence":"first","affiliation":[{"name":"Department of Radiology Second Affiliated Hospital of Chongqing Medical University  Chongqing P.R. 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