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Here, we show a metal\u2010 and complex reagent\u2010free strategy for the conversion of aldehydes to nitriles through carbamoylaldoxime intermediates. Therefore, we synthesize aldoximes from several aldehydes using hydroxylamine, which in turn are reacted with dimethylcarbamoyl chloride (DMCC) to afford\n                    <jats:italic>N,N\u2010<\/jats:italic>\n                    dimethylcarbamoyloximes. Subsequent heating cleanly produces the desired nitriles as well as volatile CO\n                    <jats:sub>2<\/jats:sub>\n                    and HNMe\n                    <jats:sub>2<\/jats:sub>\n                    through a pericyclic\n                    <jats:italic>syn<\/jats:italic>\n                    elimination. This approach relies on widely available commercial chemicals, proceeds with broad functional group tolerance, and minimizes the need for extensive purification of the nitrile product.\n                  <\/jats:p>","DOI":"10.1002\/chem.202502629","type":"journal-article","created":{"date-parts":[[2025,11,10]],"date-time":"2025-11-10T09:26:26Z","timestamp":1762766786000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Efficient, Functional Group\u2010Tolerant, and Catalyst\u2010Free Nitrile Formation from Aldehydes"],"prefix":"10.1002","volume":"31","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0210-1601","authenticated-orcid":false,"given":"Simay","family":"Aydonat","sequence":"first","affiliation":[{"name":"Department of Chemistry and Biology University of Wuppertal  Gau\u00dfstr. 20 42119 Wuppertal Germany"},{"name":"DWI \u2013 Leibniz Institute for Interactive Materials  Forckenbeckstr. 50 52056 Aachen Germany"},{"name":"Institute of Technical and Macromolecular Chemistry RWTH Aachen University  Worringerweg 2 52074 Aachen Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2815-9630","authenticated-orcid":false,"given":"Davide","family":"Campagna","sequence":"additional","affiliation":[{"name":"DWI \u2013 Leibniz Institute for Interactive Materials  Forckenbeckstr. 50 52056 Aachen Germany"},{"name":"Institute of Technical and Macromolecular Chemistry RWTH Aachen University  Worringerweg 2 52074 Aachen Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7483-6236","authenticated-orcid":false,"given":"Robert","family":"G\u00f6stl","sequence":"additional","affiliation":[{"name":"Department of Chemistry and Biology University of Wuppertal  Gau\u00dfstr. 20 42119 Wuppertal Germany"},{"name":"DWI \u2013 Leibniz Institute for Interactive Materials  Forckenbeckstr. 50 52056 Aachen Germany"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2025,11,10]]},"reference":[{"volume-title":"Pharmaceutical substances: Syntheses, Patents, Applications","year":"2001","author":"Kleemann A.","key":"e_1_2_5_1_1"},{"volume-title":"The Pesticide Manual","year":"2000","author":"Tomlin C. 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