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Herein, polymers are co\u2010crystallized with sub\u2010nm anionic metal oxide clusters (MOCs) using Li\n                    <jats:sup>+<\/jats:sup>\n                    counterions, achieving synergistic superionic conduction and mechanical robustness. Mixing MOC (Li\n                    <jats:sub>4<\/jats:sub>\n                    SiW\n                    <jats:sub>12<\/jats:sub>\n                    O\n                    <jats:sub>40<\/jats:sub>\n                    ) and poly(ethylene glycol) (PEG) affords face\u2010centered cubic crystalline structures at high MOC loadings (\u2265 60\u00a0wt.%). The crystalline framework imposes spatial nanoconfinement that favors a pronounced shift of PEG chains toward densely packed zigzag\u2010like conformations. Relaxation\u2010dynamics studies reveal substantial decoupling between Li\n                    <jats:sup>+<\/jats:sup>\n                    transport and PEG segmental relaxation, thereby enabling a superionic transport regime. The optimized composite achieves an ionic conductivity of 1.1 mS cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 110\u00b0C with an apparent activation energy of 0.32\u00a0eV. Since the long\u2010range mobility of SiW\n                    <jats:sub>12<\/jats:sub>\n                    <jats:sup>4\u2212<\/jats:sup>\n                    is constrained, the electrolyte exhibits pronounced single\u2010ion\u2010conducting character with a high lithium\u2010ion transference number (0.79). Furthermore, the composition with inorganic Li\n                    <jats:sub>4<\/jats:sub>\n                    SiW\n                    <jats:sub>12<\/jats:sub>\n                    O\n                    <jats:sub>40<\/jats:sub>\n                    enhances the mechanical modulus (25.04\u00a0MPa) and thermal stability with intrinsic flame retardancy. Solid\u2010state symmetric supercapacitors fabricated from the electrolyte exhibit predominantly electric\u2010double\u2010layer capacitive behavior with a high specific capacitance (76 F g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and excellent rate capability (87.16%).\n                  <\/jats:p>","DOI":"10.1002\/smll.75816","type":"journal-article","created":{"date-parts":[[2026,9,16]],"date-time":"2026-09-16T11:33:38Z","timestamp":1789558418000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Polymer\u2010Metal Oxide Cluster Co\u2010Crystallization for the Synergy of Superionic Conduction and Mechanical Robustness"],"prefix":"10.1002","author":[{"given":"Weigang","family":"Sun","sequence":"first","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhao","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8090-5579","authenticated-orcid":false,"given":"Lu","family":"Liu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Binghui","family":"Xue","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiadong","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuling","family":"Liang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2902-8376","authenticated-orcid":false,"given":"Panchao","family":"Yin","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Luminescent Materials and Devices &amp; South China Advanced Institute for Soft Matter Science and Technology Guangdong Basic Research Center of Excellence for Energy and Information Polymer Materials South China University of Technology  Guangzhou People's Republic of 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