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In situ biomimetic remineralization is considered a promising method, but its low efficiency is a key challenge. Additionally, the interference of cariogenic bacteria further exacerbates the problem. In this study, self\u2010assembled photothermal particles (PAEB) with light\u2010boosted synergistic biofilm eradication and remineralization properties for caries treatment are reported. Composed by polyaspartic acid\u2010stabilized amorphous calcium phosphate (Pasp\u2010ACP) and \u03b5\u2010poly\u2010L\u2010lysine\/baicalein (EPL\u2010BC), PAEB enable efficient light\u2010to\u2010heat conversion under near\u2010infrared light exposure due to polymerization and stacking of baicalein. The localized hyperthermia, accompanied with EPL\u2010BC disrupts bacterial membranes and eradicates biofilm by more than 99%, which is seven times higher than the non\u2010radiation group (12.86%) and \u224821 times higher than the fluoride group (4.35%). Meanwhile, the releasing of calcium and phosphate ions is accelerated for rapid remineralization, with highest hardness recovery (1.96\u00a0GPa) of all groups, comparable to untreated healthy enamel. Moreover, in vivo microbiome analysis confirms that PAEB selectively reduces the abundance of cariogenic\n                    <jats:italic>Streptococcus spp<\/jats:italic>\n                    . while maintaining overall microbial diversity and oral ecological balance, presenting a promising solution for non\u2010invasive dental caries treatment. This photothermal\u2010enhanced strategy gives a reference for the design of bioactive therapeutic dental materials.\n                  <\/jats:p>","DOI":"10.1002\/smll.202503224","type":"journal-article","created":{"date-parts":[[2025,6,20]],"date-time":"2025-06-20T03:18:12Z","timestamp":1750389492000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Self\u2010Assembled Photothermal Particles Boost Synergistic Biofilm Eradication and Remineralization in Early Dental Caries Treatment"],"prefix":"10.1002","volume":"21","author":[{"given":"Shiran","family":"Sun","sequence":"first","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiangwei","family":"Xin","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhengxin","family":"Ma","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wanshan","family":"Gao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Oral Diseases West China Hospital of Stomatology, Sichuan University  Chengdu 610041 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Cheng","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yihua","family":"Liu","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yijie","family":"Huang","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hongbo","family":"Zhang","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifei","family":"Yang","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiang","family":"Lin","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liwei","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Oral Diseases West China Hospital of Stomatology, Sichuan University  Chengdu 610041 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyuan","family":"Xu","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7399-3459","authenticated-orcid":false,"given":"Chunmei","family":"Ding","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianshu","family":"Li","sequence":"additional","affiliation":[{"name":"College of Polymer Science and Engineering State Key Laboratory of Advanced Polymer Materials Sichuan University  Chengdu 610065 China"},{"name":"State Key Laboratory of Oral Diseases West China Hospital of Stomatology, Sichuan University  Chengdu 610041 China"},{"name":"Med\u2010X Center for Materials Sichuan University  Chengdu 610041 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,6,20]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"crossref","first-page":"S12","DOI":"10.1111\/jcpe.12679","volume":"44","author":"Marsh P. 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