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Here, we report a bioinspired strategy that exploits the intramolecular acid\u2010base synergy of amino acids for efficient PET depolymerization. Alanine functions as a bifunctional organocatalyst, enabling complete PET esterolysis by dimethyl carbonate within 3\u00a0h at 180 \u00b0C to afford dimethyl terephthalate (98%) and ethylene carbonate (80%). Extending this concept, trace water in\n                    <jats:italic>N\u2010<\/jats:italic>\n                    methyl \u20102\u2010pyrrolidone induces in situ generation of 4\u2010(methylamino)butyric acid, which emulates amino acid bifunctionality and enables catalyst\u2010free depolymerization under identical conditions. Density functional theory (DFT) calculations reveal an intramolecular dual\u2010site acid\u2010base mechanism, where \u2013COO\n                    <jats:sup>\u2212<\/jats:sup>\n                    and \u2013NH\n                    <jats:sub>2<\/jats:sub>\n                    \u207a\u00a0groups cooperatively activate methanol and PET carbonyls through hydrogen\u2010bonded cyclic transition states, lowering the barrier by \u223c29\u00a0kcal\u00a0mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    . The method extends broadly to polyesters and polycarbonate, while establishing a transferable design paradigm that translates catalytic principles from nature into organocatalyst and solvent design, underscoring solvent molecular design as a general lever for sustainable catalysis and plastic upcycling.\n                  <\/jats:p>","DOI":"10.1002\/anie.202513723","type":"journal-article","created":{"date-parts":[[2025,9,23]],"date-time":"2025-09-23T13:33:38Z","timestamp":1758634418000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":26,"title":["From Solvent to Catalyst: In Situ Amino Acid\u2010Like Species Enable PET Upcycling Without Added Catalysts"],"prefix":"10.1002","volume":"64","author":[{"given":"Xiong","family":"Gao","sequence":"first","affiliation":[{"name":"State Key Laboratory of Soil Pollution Control and Safety Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"},{"name":"College of Environmental and Resource Sciences Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhuo","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Soil Pollution Control and Safety Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"},{"name":"College of Environmental and Resource Sciences Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Minghao","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Soil Pollution Control and Safety Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"},{"name":"College of Environmental and Resource Sciences Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunkai","family":"Yu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Soil Pollution Control and Safety Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"},{"name":"College of Environmental and Resource Sciences Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shaoyu","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Soil Pollution Control and Safety Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"},{"name":"College of Environmental and Resource Sciences Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0210-1377","authenticated-orcid":false,"given":"Qingqing","family":"Mei","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Soil Pollution Control and Safety Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"},{"name":"College of Environmental and Resource Sciences Zhejiang University  866 Yuhangtang Road Hangzhou Zhejiang 310058 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,9,23]]},"reference":[{"key":"e_1_2_6_1_1","unstructured":"OECD \u201cGlobal Plastics Outlook: Policy Scenarios to 2060\u201d can be found underhttps:\/\/www.oecd.org\/en\/publications\/global\u2010plastics\u2010outlook_aa1edf33\u2010en.html 2022."},{"key":"e_1_2_6_2_1","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.1700782"},{"key":"e_1_2_6_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-021-00648-4"},{"key":"e_1_2_6_4_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.jhazmat.2022.128816"},{"key":"e_1_2_6_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-021-00407-8"},{"key":"e_1_2_6_6_1","volume":"64","author":"Yu Y.","year":"2025","journal-title":"Angew. 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