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Nanoscale metal\u2013organic frameworks (nMOFs) based on high\u2010Z secondary building units (SBUs) and photosensitizing ligands have been developed to perform RDT. However, the rapid recombination of electron\u2013holes reduces RDT efficiency, and an abundant matrix prevents nMOFs penetration into tumors. In this study, we combine heterojunction engineering with nMOFs\u2010based RDT for the first time to prepare an Hf\u2010TCPP\/Nb\n                    <jats:sub>2<\/jats:sub>\n                    C@PEG Schottky heterojunction (HTNCP). Relying on the Nb\n                    <jats:sub>2<\/jats:sub>\n                    C's exceptional electrons absorption and photothermal conversion, HTNCP not only promotes electron\u2013hole separation in Hf\u2010TCPP, boosting superoxide radical and singlet oxygen production by 2.64\u2010fold, but also utilizes a mild photothermal effect to degrade the collagen matrix to promote self\u2010penetration. Through sequential treatment involving irradiation 1064\u00a0nm laser and X\u2010ray, HTNCP can suppress the growth and metastasis of triple\u2010negative breast cancer tumors in mice using ultra\u2010low\u2010dose X\u2010ray (1\u00a0Gy \u00d7 5). This novel radiosensitizer displays excellent RDT efficacy and provides a universal sequential treatment strategy of \u201cmatrix degradation\u2013RDT killing\u201d for clinical tumor radiotherapy.\n                  <\/jats:p>","DOI":"10.1002\/adma.202521580","type":"journal-article","created":{"date-parts":[[2026,3,8]],"date-time":"2026-03-08T17:32:31Z","timestamp":1772991151000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["A Stepwise\u2010Enhanced Schottky Heterojunction Enables Ultra\u2010Low\u2010Dose Radiodynamic Therapy via Matrix Remodeling and Electron\u2013Hole Separation"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-6022-9255","authenticated-orcid":false,"given":"Chaoyi","family":"Lyu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Advanced Medical Materials and Devices Tianjin Key Laboratory of Radiation Medicine and Molecular Nuclear Medicine Key Laboratory of Radiopharmacokinetics for Innovative Drugs Tianjin Institutes of Health Science Institute of Radiation Medicine Chinese Academy of Medical Sciences &amp; Peking Union Medical College Tianjin 300192 P. 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