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Landau theory dictates a ferroelectric\u2013paraelectric transition at Curie temperature (TC); spontaneous polarization persists below TC, while the high-symmetry paraelectric phase above TC enforces zero polarization, thus inherently eliminating the remnant polarization and hysteresis. Here, we transform common 2D ferroelectric CuInP2S6 into robust vdW dielectrics at room temperature by cationic substitution at Cu sites. The ferroelectricity is suppressed by disrupting long-range dipolar order, exhibiting hysteresis-free paraelectric behavior and preserving structural integrity and high dielectric constant. Centimeter-scale single crystals (Cu1\u2212xM\u2032xInP2S6, 0.05\u00a0\u2264\u00a0x\u00a0\u2264\u00a00.4) are exfoliable into atomically flat nanoflakes. The paraelectric Cu0.8Ag0.2InP2S6 exhibits a record-high dielectric constant (\u03ba\u00a0\u223c\u00a0108) among vdW layered dielectrics, maintaining a low leakage current (\u223c10\u221212\u00a0A) and a breakdown field of \u223c2.6\u00a0MV\/cm. These dielectrics form trap-free vdW interfaces with few-layer MoS2, enabling transistors with 0.5\u00a0V operation, 108 ON\/OFF ratio and 62\u00a0mV\/dec subthreshold swing.<\/jats:p>","DOI":"10.1093\/nsr\/nwag126","type":"journal-article","created":{"date-parts":[[2026,2,28]],"date-time":"2026-02-28T12:54:15Z","timestamp":1772283255000},"source":"Crossref","is-referenced-by-count":4,"title":["Ferroelectric-to-paraelectric phase engineering for 2D layered ultra-high-\n                    <i>\u03ba<\/i>\n                    dielectrics"],"prefix":"10.1093","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2467-630X","authenticated-orcid":false,"given":"Jianmin","family":"Yan","sequence":"first","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]},{"name":"Joint Research Center of Microelectronics, The Hong Kong Polytechnic University , Hong Kong ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jianmiao","family":"Guo","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]},{"name":"Joint Research Center of Microelectronics, The Hong Kong Polytechnic University , Hong Kong ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhihang","family":"Xu","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tianqing","family":"Wan","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]},{"name":"Joint Research Center of Microelectronics, The Hong Kong Polytechnic University , Hong Kong ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jie","family":"Li","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]},{"name":"Joint Research Center of Microelectronics, The Hong Kong Polytechnic University , Hong Kong ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Biao","family":"Zhang","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]},{"name":"Joint Research Center of Microelectronics, The Hong Kong Polytechnic University , Hong Kong ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cong","family":"Wang","sequence":"additional","affiliation":[{"name":"The Hong Kong Polytechnic University Department of Applied Physics, , Hong Kong ,","place":["China"]},{"name":"Joint Research 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