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Here we show that fluorine\u2010free poly(ionic liquid)s (PILs) operate as solid\u2010state electrolyte layers whose intrinsic electric fields modulate the competition between electrochemical hydrogenation (ECH) and the hydrogen evolution reaction (HER). When applied to Pd\u2010C catalysts, PIL binders reshape the electric double layer by repelling alkali cations and modulating interfacial pH, which change the kinetics of proton\u2010electron transfer, suppress Tafel hydrogen recombination and promotes selective coupling of adsorbed hydrogen with organic substrates. The resulting electrodes achieve up to fivefold higher ECH yields and fourfold greater Faradaic efficiencies than those based on Nafion or PVDF in three different pH values 0.6, 5.2, and 13, while simultaneously reducing Pd leaching. These findings identify the polymer additives more than a binder, but rather as an active field\u2010modulating medium. A solid analogue of the electrolyte double layer, thus extending classical electrolyte\u2010effect concepts to polymer\u2010confined interfaces and offering a strategy for binder\u2010controlled interfacial design in electrosynthetic systems.<\/jats:p>","DOI":"10.1002\/anie.2052091","type":"journal-article","created":{"date-parts":[[2026,5,20]],"date-time":"2026-05-20T15:35:58Z","timestamp":1779291358000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Programmable Solid\u2010Electrolyte Interfaces for Efficient and Selective Electrochemical Hydrogenations"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4201-1042","authenticated-orcid":false,"given":"Anastasios Orestis","family":"Grammenos","sequence":"first","affiliation":[{"name":"Colloid Chemistry Department Max Planck Institute of Colloids and Interfaces  Potsdam 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