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Heretofore, metal-based agents dominate the landscape of available magnetic resonance imaging (MRI) contrast agents and photothermal therapeutic agents, but with associated metal-specific downsides. Here, an all-organic metal-free nanoprobe, whose appreciable biocompatibility is synergistically contributed by its tetra-organo-components, is developed as a viable alternative to metal-based probes for MRI-guided tumor-targeted photothermal therapy (PTT). This rationally entails a glycol chitosan (GC)-linked polypyrrole (PP) nanoscaffold that provides abundant primary and secondary amino groups for amidation with the carboxyl groups in a nitroxide radical (TEMPO) and folic acid (FA), to obtain GC-PP@TEMPO-FA NPs. Advantageously, the appreciably benign GC-PP@TEMPO-FA features high nitroxide loading (r1 = 1.58 mM\u20131 s\u20131) and in vivo nitroxide-reduction resistance, prolonged nitroxide-systemic circulation times, appreciable water dispersibility, potential photodynamic therapeutic and electron paramagnetic resonance imaging capabilities, considerable biocompatibility, and ultimately achieves a 17 h commensurate MRI contrast enhancement. Moreover, its GC component conveys a plethora of PP to tumor sites, where FA-mediated tumor targeting enables substantial NP accumulation with consequential near-complete tumor regression within 16 days in an MRI-guided PTT. The present work therefore promotes the engineering of organic-based metal-free biocompatible NPs in synergism, in furtherance of tumor-targeted image-guided therapy.<\/jats:p>","DOI":"10.1021\/acsnano.0c09590","type":"journal-article","created":{"date-parts":[[2021,1,19]],"date-time":"2021-01-19T10:50:34Z","timestamp":1611053434000},"page":"3079-3097","source":"Crossref","is-referenced-by-count":56,"title":["Metal-Free\nOrgano-Theranostic Nanosystem with High\nNitroxide Stability and Loading for Image-Guided Targeted Tumor Therapy"],"prefix":"10.1021","volume":"15","author":[{"given":"Ozioma\nU.","family":"Akakuru","sequence":"first","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]},{"name":"University of Chinese Academy of Sciences , No. 19(A) Yuquan Road , Shijingshan District, , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen","family":"Xu","sequence":"additional","affiliation":[{"name":"University of Chinese Academy of Sciences , , ,","place":["Ningbo, China, 315010"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuang","family":"Liu","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]},{"name":"University of Chinese Academy of Sciences , No. 19(A) Yuquan Road , Shijingshan District, , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zihou","family":"Li","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Xing","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]},{"name":"University of Chinese Academy of Sciences , No. 19(A) Yuquan Road , Shijingshan District, , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunshu","family":"Pan","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanying","family":"Li","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]},{"name":"University of Chinese Academy of Sciences , No. 19(A) Yuquan Road , Shijingshan District, , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Elvis I.","family":"Nosike","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]},{"name":"University of Chinese Academy of Sciences , No. 19(A) Yuquan Road , Shijingshan District, , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhoujing","family":"Zhang","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zubair M.","family":"Iqbal","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]},{"name":"Zhejiang Sci-Tech University , , No. 2 Road of Xiasha , ,","place":["Hangzhou, China, 310018"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianjun","family":"Zheng","sequence":"additional","affiliation":[{"name":"University of Chinese Academy of Sciences , , ,","place":["Ningbo, China, 315010"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7200-8923","authenticated-orcid":true,"given":"Aiguo","family":"Wu","sequence":"additional","affiliation":[{"name":"Ningbo Institute of Materials Technology and Engineering, CAS , , 1219 ZhongGuan West Road , ,","place":["Ningbo, China, 315201"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2021,1,19]]},"reference":[{"key":"2026081810200719200_cit1","doi-asserted-by":"publisher","first-page":"401","DOI":"10.1021\/acs.biomac.8b01453","article-title":"Enhanced Photoacoustic and 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