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Intrinsically microporous polymers and conventional polymers are typically regarded as fundamentally distinct electrolyte platforms; direct comparisons between compositionally similar examples are lacking. Here, we introduce a strategy for the synthesis of fluorinated aryl sulfonimide\u2010based polymers of intrinsic microporosity (FAS\u2010PIMs) together with flexible polysulfonimide analogs of similar composition that lack permanent microporosity. Although these polymers possess fundamentally different dry\u2010state architectures, incorporation of a common pore\u2010filling transport medium, succinonitrile (SN), drives the two systems toward remarkably similar nanostructures with similar bulk conductivities (&gt;10\n                    <jats:sup>\u22125<\/jats:sup>\n                    \u201310\n                    <jats:sup>\u22124<\/jats:sup>\n                    S\/cm at 40\u00b0C\u201380\u00b0C), thermomechanical properties (\n                    <jats:italic>G<\/jats:italic>\n                    \u02b9 within 1\u201310\u00a0MPa over the temperature range of 25\u00b0C\u2013120\u00b0C), and reprocessability. Molecular dynamics simulations and experiments suggest these unusual combinations of properties arise through different conduction mechanisms within the materials, and that sulfonimide anions are particularly advantageous for conduction in microporous matrices relative to strongly binding anions. Overall, this work introduces the first sulfonimide\u2010based PIM, establishes a comparison between permanently microporous and transiently porous single\u2010ion conducting polymers, and demonstrates that these two traditionally distinct electrolyte architectures can converge toward similar, useful bulk properties after incorporation of a pore\u2010filling transport medium.\n                  <\/jats:p>","DOI":"10.1002\/anie.8257644","type":"journal-article","created":{"date-parts":[[2026,9,26]],"date-time":"2026-09-26T12:05:40Z","timestamp":1790424340000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Synthesis of Ladder and Flexible Polysulfonimides Directly From Anionic Monomers: Investigating Structure\u2013Property Convergence in Succinonitrile\u2013Polymer Electrolyte Blends"],"prefix":"10.1002","author":[{"given":"Abraham","family":"Herzog\u2010Arbeitman","sequence":"first","affiliation":[{"name":"Department of Chemistry Massachusetts Institute of Technology  Cambridge Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Pablo","family":"Leon","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Massachusetts Institute of Technology  Cambridge Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Benedikt S.","family":"Schreib","sequence":"additional","affiliation":[{"name":"Department of Chemistry Massachusetts Institute of Technology  Cambridge Massachusetts USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1974-028X","authenticated-orcid":false,"given":"KyuJung","family":"Jun","sequence":"additional","affiliation":[{"name":"Department of Materials Science and Engineering Massachusetts Institute 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