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However, monolayer or few\u2010layered 2D magnets are not yet realized, even though a wide spectrum of 2D Ruddlesden\u2013Popper (RP) OIHPs are known as quasi\u20102D Heisenberg magnets in bulk compounds. Here, chemical exfoliation by solvent engineering is applied to successfully synthesize large\u2010sized, few unit\u2010cell\u2010thick 2D RP\u2010OIHPs. Comprehensive structural characterization reveals that binary co\u2010solvents with high relative polarity in spin coating technique are the most effective among nine kinds of solvents. Above all, this enables few\u2010layered 2D RP\u2010OIHP ultrathin films sustaining their intrinsic magnetic order. It is found that XY\u2010like magnetic anisotropy driven by Jahn\u2013Teller effect responsible for ferromagnetism in seven\u2010layered (C<jats:sub>6<\/jats:sub>H<jats:sub>5<\/jats:sub>CH<jats:sub>2<\/jats:sub>CH<jats:sub>2<\/jats:sub>NH<jats:sub>3<\/jats:sub>)<jats:sub>2<\/jats:sub>CuCl<jats:sub>4<\/jats:sub> ultrathin films remains very robust, whereas Ising\u2010like dipolar anisotropy responsible for canted antiferromagnetism in ten\u2010layered (C<jats:sub>6<\/jats:sub>H<jats:sub>5<\/jats:sub>CH<jats:sub>2<\/jats:sub>CH<jats:sub>2<\/jats:sub>NH<jats:sub>3<\/jats:sub>)<jats:sub>2<\/jats:sub>MnCl<jats:sub>4<\/jats:sub> ultrathin films is greatly reduced. It is expected that ferromagnetism even at monolayer limit should be possible by means of further sophisticated solvent engineering as long as Jahn\u2013Teller effect is active. The chemical exfoliation using solvent engineering unambiguously can bring about a new breakthrough in the development of 2D RP\u2010OIHP van der Waals magnets for ultrahigh energy\u2010efficient spintronic, opto\u2010spintronic devices.<\/jats:p>","DOI":"10.1002\/smll.202005445","type":"journal-article","created":{"date-parts":[[2020,11,26]],"date-time":"2020-11-26T09:46:24Z","timestamp":1606383984000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":17,"title":["Intrinsic Magnetic Order of Chemically Exfoliated 2D Ruddlesden\u2013Popper Organic\u2013Inorganic Halide Perovskite Ultrathin Films"],"prefix":"10.1002","volume":"16","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0672-2915","authenticated-orcid":false,"given":"Ki\u2010Yeon","family":"Kim","sequence":"first","affiliation":[{"name":"Quantum Beam Science Division Korea Atomic Energy Research Institute  Daejeon 34057 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Garam","family":"Park","sequence":"additional","affiliation":[{"name":"Nuclear Chemistry Research Team Korea Atomic Energy Research Institute  Daejeon 34057 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jaehun","family":"Cho","sequence":"additional","affiliation":[{"name":"Division of Nanotechnology Daegu Gyeongbuk Institute of Science and Technology (DGIST)  Daegu 42988 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Joonwoo","family":"Kim","sequence":"additional","affiliation":[{"name":"Division of Nanotechnology Daegu Gyeongbuk Institute of Science and Technology (DGIST)  Daegu 42988 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"June\u2010Seo","family":"Kim","sequence":"additional","affiliation":[{"name":"Division of Nanotechnology Daegu Gyeongbuk Institute of Science and Technology (DGIST)  Daegu 42988 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinyong","family":"Jung","sequence":"additional","affiliation":[{"name":"Department of Emerging Materials Science Daegu Gyeongbuk Institute of Science and Technology (DGIST)  Daegu 42988 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kwonjin","family":"Park","sequence":"additional","affiliation":[{"name":"Department of Emerging Materials Science Daegu Gyeongbuk Institute of Science and Technology (DGIST)  Daegu 42988 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chun\u2010Yeol","family":"You","sequence":"additional","affiliation":[{"name":"Department of Emerging Materials Science Daegu Gyeongbuk Institute of Science and Technology (DGIST)  Daegu 42988 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"In\u2010Hwan","family":"Oh","sequence":"additional","affiliation":[{"name":"Quantum Beam Science Division Korea Atomic Energy Research Institute  Daejeon 34057 Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2020,11,26]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1039\/C7CS00288B"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.aav4450"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.6b03052"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature22060"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature22391"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565-018-0063-9"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.8b00683"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.17.1133"},{"key":"e_1_2_7_9_1","first-page":"493","volume":"32","author":"Berezinskii V.","year":"1971","journal-title":"Sov. 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