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But this requires ultrathin nanoplatelets with three or fewer monolayers of PbI\n                    <jats:sub>6<\/jats:sub>\n                    octahedra across the thickness, which are challenging to synthesise uniformly, and their luminescence is strongly affected by surface defects. Together, these limit the performance of ultrathin PeNPLs in light\u2010emitting diodes (LEDs). Here, we address these challenges with an ancillary ligand engineering strategy. We demonstrate that ligands with phosphoryl functional groups strongly bind to the perovskite surface, while having an organic backbone that is not sterically bulky ensures high ligand density. By modulating nucleation and growth, these ancillary ligands lead to monodisperse PeNPLs that stack more uniformly when self\u2010assembled into superlattices, with suppressed agglomeration. As a result, from edge\u2010up PeNPL superlattices, we achieve an enhanced degree of polarization, while from face\u2010down PeNPL superlattices, we achieve enhanced outcoupling that results in LEDs with 13.1% external quantum efficiency, the highest reported for ultrathin PeNPL LEDs. This work establishes ancillary ligand\u2010induced synthesis as a decisive route to achieve uniform nanoplatelets with robust orientation control, enabling full utilization of the multifunctionality of anisotropic PeNPLs.\n                  <\/jats:p>","DOI":"10.1002\/adma.74023","type":"journal-article","created":{"date-parts":[[2026,7,10]],"date-time":"2026-07-10T13:02:02Z","timestamp":1783688522000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Ligand Engineering for Precise Control of Ultrathin CsPbI\n                    <sub>3<\/sub>\n                    Nanoplatelet Superlattices for Efficient Light\u2010Emitting Diodes"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0009-0003-4931-1950","authenticated-orcid":false,"given":"Jongbeom","family":"Kim","sequence":"first","affiliation":[{"name":"Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST)  Ulsan Republic of Korea"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Woo Hyeon","family":"Jeong","sequence":"additional","affiliation":[{"name":"School of Advanced Materials Science and Engineering Sungkyunkwan University  Suwon Republic of Korea"},{"name":"Inorganic Chemistry Laboratory University of Oxford  Oxford UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8919-9236","authenticated-orcid":false,"given":"Junzhi","family":"Ye","sequence":"additional","affiliation":[{"name":"Inorganic Chemistry Laboratory University of Oxford  Oxford UK"},{"name":"Institute of Polymer Optoelectronic Materials and Devices Guangdong Basic Research Center of Excellence for Energy &amp; 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