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Despite extensive interest, however, organosilicon ferroelectric crystals have never been found. Here, by using the chemical design strategy, we successfully obtained a molecular ferroelectric D\u2010<jats:italic>chiro<\/jats:italic>\u2010inositol\u2010SiMe<jats:sub>3<\/jats:sub> with polar <jats:italic>P<\/jats:italic>4<jats:sub>3<\/jats:sub> symmetry, whose spontaneous polarization can be electrically switchable on thin film. The introduction of organosilicon groups endows the thin films with excellent softness, ductility and flexibility (extremely low hardness of 72.8\u2005MPa and small elastic modulus of 5.04\u2005GPa) that are desirable for biomedical and human\u2010compatible applications. As the first case of organosilicon ferroelectric crystal to date, this work offers a new structural paradigm for molecular ferroelectrics, and highlights their potential for flexible bio\u2010electronic applications.<\/jats:p>","DOI":"10.1002\/anie.202210809","type":"journal-article","created":{"date-parts":[[2022,9,14]],"date-time":"2022-09-14T15:13:01Z","timestamp":1663168381000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":32,"title":["The First Chiro\u2010Inositol Organosilicon Ferroelectric Crystal"],"prefix":"10.1002","volume":"61","author":[{"given":"Zhi\u2010Xu","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Bioelectronics Southeast University  Nanjing 211189 P. R. 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