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However, challenges such as low Curie temperatures (T\n                    <jats:italic>\n                      <jats:sub>C<\/jats:sub>\n                    <\/jats:italic>\n                    ) and ambient instability have hindered their practical applications. In this study, we employ chemical vapor deposition (CVD) combined with salt\u2010assisted methods and optimize growth parameters to synthesize phase\u2010tunable Cr\n                    <jats:sub>x<\/jats:sub>\n                    S\n                    <jats:sub>y<\/jats:sub>\n                    compounds, including rhombohedral Cr\n                    <jats:sub>2<\/jats:sub>\n                    S\n                    <jats:sub>3<\/jats:sub>\n                    (ferrimagnetic below 120 K), trigonal Cr\n                    <jats:sub>5<\/jats:sub>\n                    S\n                    <jats:sub>6<\/jats:sub>\n                    (room\u2010temperature ferrimagnetic), and hexagonal CrS (antiferromagnetic). Our findings reveal that self\u2010intercalation of Cr atoms significantly modifies the lattice structure, electronic states, and magnetic properties of these materials. Cr\n                    <jats:sub>5<\/jats:sub>\n                    S\n                    <jats:sub>6<\/jats:sub>\n                    exhibits half\u2010metallic characteristics with room\u2010temperature ferrimagnetism, representing a significant advancement for practical 2D magnetic materials. The charge transfer from self\u2010intercalated Cr atoms and superexchange interactions mediated by sulfur\n                    <jats:italic>p<\/jats:italic>\n                    \u2010orbitals are identified as key mechanisms driving these tunable properties. This work highlights self\u2010intercalation as a transformative strategy for engineering high\u2010performance 2D magnetic materials, providing insights for advancing next\u2010generation spintronic devices.\n                  <\/jats:p>","DOI":"10.1002\/smll.202514047","type":"journal-article","created":{"date-parts":[[2026,2,11]],"date-time":"2026-02-11T07:55:46Z","timestamp":1770796546000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Self\u2010Intercalated CrxSy: 2D Ferrimagnetic Materials From Low\u2010Temperature to Room\u2010Temperature"],"prefix":"10.1002","volume":"22","author":[{"given":"Bicheng","family":"Wang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Yao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenting","family":"Hong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xu","family":"He","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chuanyong","family":"Jian","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhaoan","family":"Hong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qian","family":"Cai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Functional Crystals and Devices Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences  Fuzhou Fujian P. R. 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