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To address these challenges, we report a design concept for pyrrolidone\u2010based star\u2010polyamides synthesized from itaconic acid and cadaverine, whose architecture provides exceptional sensitivity to external stimuli. In a stark departure from the classical Hofmeister series, Ca\n                    <jats:sup>2+<\/jats:sup>\n                    initiates an anomalous salting\u2010in effect that contrasts with the Na\n                    <jats:sup>+<\/jats:sup>\n                    \u2010induced salting\u2010out. DFT\/MD calculations reveal that pyrrolidone moderately coordinates with Ca\n                    <jats:sup>2+<\/jats:sup>\n                    without disrupting its hydration shell, thereby imparting a dense positive charge to the coacervate surfaces. Crucially, the cationic surface charge endows the coacervates with light\u2010scattering bodies with superior dispersion stability, surpassing conventional PNIPAM by over 20\u2010fold. The system maintains robust stability at 5\u00a0mol\/L, a regime where conventional thermoresponsive polymers inevitably fail. An applied electric field enables spatial control of transparency, creating a dual electro\u2010thermal responsive system for energy\u2010efficient, sustainable smart windows. Furthermore, the Ca\n                    <jats:sup>2+<\/jats:sup>\n                    salting\u2010in effects enable coacervation in a high polymer concentration range over 50% to establish pseudosolidity, which provides a versatile platform for next\u2010generation electro\u2010thermal soft systems, ranging from implantable biosensors to battery\u2010operated smart windows.\n                  <\/jats:p>","DOI":"10.1002\/advs.78227","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T04:00:27Z","timestamp":1791777627000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Ionically Counter\u2010Programmable Phase\u2010Separation of Superstable Star\u2010Biopolyamide Coacervates for Electrothermally\u2010Responsive Pseudosolid Smart Windows"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0007-5908-0411","authenticated-orcid":false,"given":"Jie","family":"Liu","sequence":"first","affiliation":[{"name":"The Key Laboratory of Synthetic and Biological Colloids School of Chemical and Material Engineering Ministry of Education Jiangnan University  Wuxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaotian","family":"Zhu","sequence":"additional","affiliation":[{"name":"The Key Laboratory of Synthetic and Biological Colloids School of Chemical and Material Engineering Ministry of Education Jiangnan University  Wuxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-3250-0813","authenticated-orcid":false,"given":"Jinjian","family":"Hou","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering Hainan University  Haikou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-8195-8768","authenticated-orcid":false,"given":"Jinze","family":"Du","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering Tianjin University  Tianjin China"},{"name":"Zhejiang Institute of Tianjin University  Ningbo China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5717-5659","authenticated-orcid":false,"given":"Mohammad Asif","family":"Ali","sequence":"additional","affiliation":[{"name":"The Key Laboratory of Synthetic and Biological Colloids School of Chemical and Material Engineering Ministry of Education Jiangnan University  Wuxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0005-6145-6532","authenticated-orcid":false,"given":"Maiko K.","family":"Okajima","sequence":"additional","affiliation":[{"name":"The Key Laboratory of Synthetic and Biological Colloids School of Chemical and Material Engineering Ministry of Education Jiangnan University  Wuxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9794-083X","authenticated-orcid":false,"given":"Tatsuo","family":"Kaneko","sequence":"additional","affiliation":[{"name":"The Key Laboratory of Synthetic and Biological Colloids School of Chemical and Material Engineering Ministry of Education Jiangnan University  Wuxi China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,11]]},"reference":[{"key":"e_1_2_10_2_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.abg0291"},{"key":"e_1_2_10_3_1","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.201902066"},{"key":"e_1_2_10_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.apenergy.2017.11.039"},{"key":"e_1_2_10_5_1","doi-asserted-by":"crossref","first-page":"1707","DOI":"10.1016\/j.joule.2018.06.018","article-title":"Thermochromic VO2 for Energy\u2010Efficient Smart Windows","volume":"2","author":"Cui 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