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Here, we report a complementary strategy that inverts the traditional design logic: starting from a magnetic metal, we induce a controlled metal\u2010to\u2010insulator transition (MIT) through dimensionality reduction in two\u2010dimensional (2D) layers. Using rhombohedral (r\u2010)Cr\n                    <jats:sub>2<\/jats:sub>\n                    Se\n                    <jats:sub>3<\/jats:sub>\n                    as a model system, we show that thinning from bulk to atomically thin nanosheets progressively opens a bandgap while preserving antiferromagnetic ordering. Transport measurements reveal a pronounced thickness\u2010dependent crossover from metallic to semiconducting behavior, driven primarily by quantum confinement under dimensional reduction, while the effects of external magnetic and electric fields remain minor. Supported by first\u2010principles calculations, our results establish r\u2010Cr\n                    <jats:sub>2<\/jats:sub>\n                    Se\n                    <jats:sub>3<\/jats:sub>\n                    as a rare non\u2010van der Waals 2D antiferromagnetic semiconductor and illustrate that dimensionality\u2010driven MIT offers a viable pathway for engineering robust 2D magnetic semiconductors, providing a new platform for spintronic and multifunctional device applications.\n                  <\/jats:p>","DOI":"10.1002\/adma.202519677","type":"journal-article","created":{"date-parts":[[2025,12,29]],"date-time":"2025-12-29T07:41:21Z","timestamp":1766994081000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Dimensionality\u2010Driven Metal\u2010to\u2010Insulator Transition in Two\u2010Dimensional Antiferromagnetic R\u2010Cr\n                    <sub>2<\/sub>\n                    Se\n                    <sub>3<\/sub>"],"prefix":"10.1002","volume":"38","author":[{"given":"Yuncheng","family":"Mu","sequence":"first","affiliation":[{"name":"School of Materials Shenzhen Campus of Sun Yat\u2010Sen University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chengzhi","family":"Li","sequence":"additional","affiliation":[{"name":"School of Materials Shenzhen Campus of Sun Yat\u2010Sen University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1506-8924","authenticated-orcid":false,"given":"Shu","family":"Zhou","sequence":"additional","affiliation":[{"name":"School of Materials Shenzhen Campus of Sun Yat\u2010Sen University  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fuhao","family":"Xue","sequence":"additional","affiliation":[{"name":"School of Materials Shenzhen Campus of Sun Yat\u2010Sen University  Shenzhen 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