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Enhancing long\u2010term memory (LTM) retention often requires enhanced ion accessibility, which can induce excessive ion accumulation and increase energy consumption. Herein, we resolve this physical dilemma by rationally engineering the spatial architecture of a poly(maleic acid)\u2010poly(styrenesulfonate) (PMA\u2010PSS) copolymer electrolyte. The density of the bulky, hydrophilic PSS blocks is increased to impose steric hindrance and thermodynamic mismatch against TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    ions, thereby limiting excessive ion influx while preserving the injected ions through a confined ion\u2013polymer coupling pathway. Such spatial confinement triggers a localized, persistent doping\u2010induced lattice expansion. This structural reorganization establishes a structural basis for suppressed TFSI\n                    <jats:sup>\u2212<\/jats:sup>\n                    back\u2010diffusion by creating a sterically constrained ion\u2013polymer environment that stabilizes the doped state. Consequently, the minimized excessive ion accumulation and suppressed post\u2010pulse ion back\u2010diffusion enable the high\u2010PSS\u2010content EGSTs to achieve exceptional LTM retention, low energy consumption, and endurance over 8,000 programming cycles. System\u2010level simulations reveal an image recognition accuracy of 87%, comparable to that of an ideal weight\u2010update model, confirming that our polyanion\u2010induced structural reorganization provides a promising blueprint for next\u2010generation, high\u2010fidelity artificial intelligence hardware.\n                  <\/jats:p>","DOI":"10.1002\/smll.75766","type":"journal-article","created":{"date-parts":[[2026,9,12]],"date-time":"2026-09-12T07:00:19Z","timestamp":1789196419000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Decoupling the Retention\u2013Energy Trade\u2010Off Through Structural Reorganization of Synaptic Polyelectrolytes for Nonvolatile Neuromorphic Devices"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-0721-7039","authenticated-orcid":false,"given":"Donghwa","family":"Lee","sequence":"first","affiliation":[{"name":"Department of Chemical and Biomolecular 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