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Recent advances in ferroelectrochemistry have provided efficient synthetic strategies to tailor these properties, with a focus on functionalizing organic components. However, the impact of combined molecular symmetry and geometry on ferroelectricity remains less understood. In this work, we construct a series of one\u2010dimensional ferroelectric hybrid metal halides (HMHs) using C\n                    <jats:sub>3v<\/jats:sub>\n                    \u2010symmetric trigonal pyramidal polar cations to systematically investigate how molecular symmetry and geometry modulate ferroelectric behavior. The model compound (TMS)PbI\n                    <jats:sub>3<\/jats:sub>\n                    (TMS\u00a0=\u00a0trimethylsulfonium) exhibits ferroelectricity up to its decomposition temperature (530\u00a0K), the highest among known HMH ferroelectrics, alongside an exceptionally low\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>c<\/jats:sub>\n                    (0.25\u00a0kV cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    at 298\u00a0K). We demonstrate that the unique C\n                    <jats:sub>3v<\/jats:sub>\n                    symmetry and trigonal pyramidal geometry of the TMS cation facilitate energy\u2010favorable uniaxial rotation about the polar 3\u2010fold axis and 90\u00b0 polarity flipping during disordering in the ferroelectric\u2013ferroelectric phase transition near 271\u00a0K. This partial disorder transition underpins the remarkable high\u2010temperature ferroelectric phase and low\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>c<\/jats:sub>\n                    . Selenium\u2010 and phosphorus\u2010based analogs show similar properties with\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>c<\/jats:sub>\n                    values of 0.55 and 0.47\u00a0kV cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    , respectively.\n                  <\/jats:p>","DOI":"10.1002\/anie.202523302","type":"journal-article","created":{"date-parts":[[2025,11,24]],"date-time":"2025-11-24T06:37:43Z","timestamp":1763966263000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Molecular Symmetry and Geometry Engineering for High\u2010Temperature Ferroelectricity and Low Coercive Field in Hybrid Metal Halides"],"prefix":"10.1002","volume":"65","author":[{"given":"Shu\u2010Yin","family":"Jia","sequence":"first","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chao\u2010Yang","family":"Chai","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiang\u2010Qiang","family":"Bi","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Bin","family":"Fu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Thorium Energy Shanghai Institute of Applied Physics Chinese Academy of Sciences  Shanghai 201800 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng\u2010Dong","family":"Liu","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ming\u2010Liang","family":"Jin","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing\u2010Meng","family":"Zhang","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wei","family":"Wang","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jia\u2010Hang","family":"Wu","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rui","family":"Zuo","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fei\u2010Yang","family":"Li","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9400-9740","authenticated-orcid":false,"given":"Wen","family":"Zhang","sequence":"additional","affiliation":[{"name":"Jiangsu Key Laboratory for Science and Applications of Molecular Ferroelectrics and School of Chemistry and Chemical Engineering Southeast University  Nanjing 211189 China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2025,11,23]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1093\/acprof:oso\/9780198507789.001.0001"},{"key":"e_1_2_7_2_1","volume-title":"Ferroelectrics and related materials","author":"Smolenskii G. 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