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Particularly, the van der Waals (vdW) gap holds promise for effective magnetic anisotropy modulation. However, the microscopic mechanisms remain elusive. Here, it is demonstrated that epitaxial growth of \u03b1\u2010Al\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>3<\/jats:sub>\n                    \/Fe\n                    <jats:sub>4<\/jats:sub>\n                    GeTe\n                    <jats:sub>2<\/jats:sub>\n                    induces a pronounced expansion of the vdW gap (up to 0.51 \u00c5) at the interface, leading to a robust enhancement of in\u2010plane magnetic anisotropy (IMA) and suppression of the spin reorientation temperature (\n                    <jats:italic>T<\/jats:italic>\n                    <jats:sub>SR<\/jats:sub>\n                    ) from 288 K to undetectable levels. This counterintuitive behavior contrasts with conventional thickness\u2010dependent perpendicular magnetic anisotropy (PMA). Combined experimental and theoretical analyses reveal that vdW gap expansion reduces Te p\n                    <jats:sub>x<\/jats:sub>\n                    \/p\n                    <jats:sub>y<\/jats:sub>\n                    orbital overlap, diminishing their contribution to magnetocrystalline anisotropy energy and suppressing PMA. These findings establish interface gap engineering as a novel route for tailoring magnetic anisotropy in 2D FMs, advancing the design of next\u2010generation spintronic devices.\n                  <\/jats:p>","DOI":"10.1002\/advs.202509941","type":"journal-article","created":{"date-parts":[[2025,12,13]],"date-time":"2025-12-13T01:54:12Z","timestamp":1765590852000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Magnetic Anisotropy Modulation via van der Waals Gap Engineering in 2D Ferromagnet Fe\n                    <sub>4<\/sub>\n                    GeTe\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"13","author":[{"given":"Weiran","family":"Xie","sequence":"first","affiliation":[{"name":"Fert Beijing Institute School of Integrated Circuit Science and Engineering Beihang University  Beijing 100191 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