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Here, using first-principles calculations and Monte Carlo simulations, we identify planar rectangular monolayer VN as an itinerant ferromagnet with an out-of-plane easy axis and an equilibrium Curie temperature of about 420\u00a0K. At equilibrium, the rectangular crystal field polarizes the dxz\/dyz doublet, producing a direction-resolved exchange network in which strong ferromagnetic Ja and diagonal Jab couplings coexist with an antiferromagnetic Jb channel. By tuning the lattice parameter b at fixed a, the rectangular field is continuously varied through the square geometry, driving a dxz-to-dyz orbital-pseudospin reversal. This orbital redistribution converts Jb from antiferromagnetic to ferromagnetic and reconstructs the competing exchange topology into a cooperative ferromagnetic network, raising TC to a broad plateau around 490\u00a0K, corresponding to an enhancement of about 18%. Orbital-resolved ICOHP analysis shows that the static V\u2013N bonding and the pz-mediated \u03c0 channel weaken overall under b-axis tuning, ruling out bond strengthening as the origin of the exchange enhancement. These results establish rectangular-distortion-driven orbital-pseudospin switching as a microscopic mechanism for engineering robust above-room-temperature ferromagnetism in two-dimensional metallic magnets.<\/jats:p>","DOI":"10.1063\/5.0349967","type":"journal-article","created":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T10:53:11Z","timestamp":1791456791000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Orbital-pseudospin switching reconstructs the competing exchange network in monolayer VN"],"prefix":"10.1063","volume":"165","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-3425-8911","authenticated-orcid":false,"given":"Kairu","family":"Dou","sequence":"first","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]},{"name":"College of Big Data and Information Engineering, Guizhou University 2 , Guiyang 550025,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nanjing","family":"Zheng","sequence":"additional","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiayu","family":"Li","sequence":"additional","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Gao","sequence":"additional","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8515-1136","authenticated-orcid":false,"given":"Qiong","family":"Peng","sequence":"additional","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0987-1622","authenticated-orcid":false,"given":"Xiaosi","family":"Qi","sequence":"additional","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1346-5280","authenticated-orcid":false,"given":"Jin","family":"Zhao","sequence":"additional","affiliation":[{"name":"Department of Physics, University of Science and Technology of China 3 , 230026 Hefei, Anhui,","place":["China"]},{"name":"Hefei National Laboratory, University of Science and Technology of China 4 , 230088 Hefei, Anhui,","place":["China"]},{"name":"CQD\/Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China 5 , 230026 Hefei, Anhui,","place":["China"]},{"name":"Department of Physics and Astronomy, University of Pittsburgh 6 , Pittsburgh, Pennsylvania 15260,","place":["USA"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-7737-7234","authenticated-orcid":false,"given":"Junfei","family":"Ding","sequence":"additional","affiliation":[{"name":"College of Physics, Guizhou Province Key Laboratory for Photoelectrics Technology and Application, Guizhou University 1 , Guiyang City 550025,","place":["People\u2019s Republic of China"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,10,8]]},"reference":[{"key":"2026100806530722000_c1","doi-asserted-by":"publisher","first-page":"265","DOI":"10.1038\/nature22060","article-title":"Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals","volume":"546","year":"2017","journal-title":"Nature"},{"key":"2026100806530722000_c2","doi-asserted-by":"publisher","first-page":"270","DOI":"10.1038\/nature22391","article-title":"Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit","volume":"546","year":"2017","journal-title":"Nature"},{"key":"2026100806530722000_c3","doi-asserted-by":"publisher","first-page":"1133","DOI":"10.1103\/PhysRevLett.17.1133","article-title":"Absence of ferromagnetism or antiferromagnetism in one- or two-dimensional isotropic Heisenberg models","volume":"17","year":"1966","journal-title":"Phys. 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