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Using a selenium-containing polypeptide platform, we constructed a nucleoside-functionalized RHP library incorporating nucleoside, cationic, and anionic interaction motifs. Machine-learning-assisted optimization of this library identified a lead RHP, termed IDP-IMP (intrinsically disordered protein-inspired immunomodulatory polypeptide), that suppresses CpG DNA\u2013Toll-like receptor 9 (TLR9) signaling with limited cytotoxicity. Rather than acting as a conventional strong nucleic acid scavenger or TLR9 antagonist, IDP-IMP showed moderate binding\/association with both CpG and TLR9 through different side chain compositions, leading to reduced intracellular CpG\u2013TLR9 colocalization. Across the polymer library, stronger CpG binding did not necessarily correspond to greater inhibitory activity, indicating that CpG binding alone did not predict functional activity. In a collagen-induced arthritis rat model, IDP-IMP attenuated inflammation and joint pathology without detectable systemic toxicity. These findings demonstrate a high-throughput approach for identifying statistical polymer compositions perturbing CpG\u2013TLR9 signaling. The results highlight the importance of IDP-like weak, multivalent, and dynamic interactions in immunomodulation.<\/jats:p>","DOI":"10.1021\/jacs.6c17839","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T16:02:46Z","timestamp":1791388966000},"page":"45193-45206","source":"Crossref","is-referenced-by-count":0,"title":["Random\nHybrid Polypeptides Regulate Immune Signaling\nthrough Promiscuous and Dynamic Interaction Landscapes"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-3055-6042","authenticated-orcid":true,"given":"Haolin","family":"Chen","sequence":"first","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]},{"name":"Sun Yat-Sen University , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haisen","family":"Zhou","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9974-2041","authenticated-orcid":true,"given":"Tianyi","family":"Jin","sequence":"additional","affiliation":[{"name":"California Institute of Technology , , , ,","place":["Pasadena, California, United States, 91125"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhihui","family":"Zhang","sequence":"additional","affiliation":[{"name":"Sun Yat-Sen University , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhenzhong","family":"Zhao","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoran","family":"Cai","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaoman","family":"Yu","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0350-7475","authenticated-orcid":true,"given":"Hong","family":"Liu","sequence":"additional","affiliation":[{"name":"Henan University , , ,","place":["Zhengzhou, China, 450046"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shi","family":"Chen","sequence":"additional","affiliation":[{"name":"Sun Yat-Sen University , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuang","family":"Li","sequence":"additional","affiliation":[{"name":"Sun Yat-Sen University , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0890-0340","authenticated-orcid":true,"given":"Xuehai","family":"Yan","sequence":"additional","affiliation":[{"name":"Institute of Process Engineering, Chinese Academy of Sciences, University of Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9763-6982","authenticated-orcid":true,"given":"Guangqi","family":"Wu","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2232-8739","authenticated-orcid":true,"given":"Miao","family":"Qi","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6133-4977","authenticated-orcid":true,"given":"Lixin","family":"Liu","sequence":"additional","affiliation":[{"name":"Sun Yat-Sen University , , ,","place":["Guangzhou, China, 510006"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongming","family":"Chen","sequence":"additional","affiliation":[{"name":"Sun Yat-Sen University , , ,","place":["Guangzhou, China, 510006"]},{"name":"Henan University , , ,","place":["Zhengzhou, China, 450046"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2180-3091","authenticated-orcid":true,"given":"Hua","family":"Lu","sequence":"additional","affiliation":[{"name":"Peking University , , ,","place":["Beijing, China, 100871"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,7]]},"reference":[{"issue":"1","key":"2026102111084969300_cit1","doi-asserted-by":"publisher","first-page":"2","DOI":"10.1016\/j.tibs.2007.10.003","article-title":"Fuzzy complexes: polymorphism and structural disorder\nin protein\u2013protein interactions","volume":"33","author":"Tompa","year":"2008","journal-title":"Trends\nBiochem. 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