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The ferroelectricity in vdW materials recently attracts renewed interest for the potential use in high\u2010density storage devices. With the thickness becoming thinner, the competition between the surface energy, depolarization field, and interfacial chemical bonds may give rise to the modification of ferroelectricity and crystalline structure, which has limited investigations. In this work, combining the piezoresponse force microscope scanning, contact resonance imaging, the existence of the intrinsic in\u2010plane polarization in vdW ferroelectrics CuInP<jats:sub>2<\/jats:sub>S<jats:sub>6<\/jats:sub> single crystals is reported, whereas below a critical thickness between 90 and 100 nm, the in\u2010plane polarization disappears. The Young's modulus also shows an abrupt stiffness at the critical thickness. Based on the density functional theory calculations, these behaviors are ascribed to a structural phase transition from monoclinic to trigonal structure, which is further verified by transmission electron microscope technique. These findings demonstrate the foundational importance of structural phase transition for enhancing the rich functionality and broad utility of vdW ferroelectrics.<\/jats:p>","DOI":"10.1002\/smll.201904529","type":"journal-article","created":{"date-parts":[[2019,12,3]],"date-time":"2019-12-03T11:31:49Z","timestamp":1575372709000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":111,"title":["Thickness\u2010Dependent In\u2010Plane Polarization and Structural Phase Transition in van der Waals Ferroelectric CuInP<sub>2<\/sub>S<sub>6<\/sub>"],"prefix":"10.1002","volume":"16","author":[{"given":"Jianming","family":"Deng","sequence":"first","affiliation":[{"name":"School of Aerospace Engineering Beijing Institute of Technology  Beijing 100081 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanyu","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Aerospace Engineering Beijing Institute of 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