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Metal thiophosphates (MTPs) with mobile Cu\n                    <jats:sup>+<\/jats:sup>\n                    ions exhibit a ferroionic state, where polarization arises from ionic redistribution among multiple nearly degenerate sites. CuVP\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>6<\/jats:sub>\n                    uniquely combines intrinsic ferromagnetism from the V sublattice with Cu\n                    <jats:sup>+<\/jats:sup>\n                    \u2010driven ferroionic configurational freedom, enabling direct exploration of how ionic dynamics influence magnetic interactions. Herein, high\u2010quality CuVP\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>6<\/jats:sub>\n                    single crystals are synthesized, and their structural and physical properties are systematically investigated. Temperature\u2010dependent neutron diffraction elucidates a ferroionic structure with dynamic distributions of copper ions across multiple crystallographic sites. The versatile occupations are driven by local symmetry\u2010controlled orbital interactions between copper ions and surrounding ligands through a second\u2010order Jahn\u2013Teller mechanism. Magnetic measurements identify a ferromagnetic (FM) transition below 3.3\u00a0K. The pressure\u2010controlled magnetocrystalline anisotropy and interlayer exchange interactions mediated by Cu\n                    <jats:sup>+<\/jats:sup>\n                    migration are demonstrated, boosting the Curie temperature remarkably by over 60% and inducing a soft\u2010to\u2010hard FM transition unparalleled within the MTP family. These results demonstrate that ionic configurational freedom provides an efficient route to control magnetism, opening new possibilities for spintronic applications.\n                  <\/jats:p>","DOI":"10.1002\/adma.202520850","type":"journal-article","created":{"date-parts":[[2026,2,10]],"date-time":"2026-02-10T11:41:52Z","timestamp":1770723712000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cu\n                    <sup>+<\/sup>\n                    \u2010Driven Ferroionic Structure and Pressure\u2010Tunable Magnetism in Layered Thiophosphate CuVP\n                    <sub>2<\/sub>\n                    S\n                    <sub>6<\/sub>"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-0503-1168","authenticated-orcid":false,"given":"Ruichen","family":"Xie","sequence":"first","affiliation":[{"name":"State Key Laboratory For Artificial Microstructure &amp; Mesoscopic Physics School of Physics Peking University  Beijing P. 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