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Here, we establish arm\u00a0length control as a central structural parameter that governs both the optical properties of individual CsPbBr\n                    <jats:sub>3<\/jats:sub>\n                    NCs and their self\u2010assembly behavior. Armed NCs, featuring a cubic core with multiple protruding arms, are synthesized by controlling seed size, concentration, and injection temperature, while arm length is tuned via cesium oleate concentration. Prolonged storage in toluene is shown to lead to a time\u2010dependent morphological evolution from armed NCs to 26\u2010faceted rhombicuboctahedra, with short\u2010armed structures as intermediates. NCs with a longer arm length yield enhanced radiative efficiency, extended photoluminescence (PL) lifetimes, and suppressed blinking, making such NCs suitable for light\u2010emitting devices and quantum photonic applications. In contrast, short\u2010armed NCs exhibit faster recombination, stronger PL intermittency, and increased surface accessibility, which are favorable for sensing and high\u2010speed single\u2010photon emission. The arm length also governs self\u2010assembly behavior, hereby opening new possibilities for applications. Armed NCs form densely 3D\u2010packed assemblies with tunable configurations. This work demonstrates how arm length tuning expands the functional potential of CsPbBr\n                    <jats:sub>3<\/jats:sub>\n                    NCs by linking morphological control to both optical response and self\u2010assembly characteristics.\n                  <\/jats:p>","DOI":"10.1002\/adma.202519211","type":"journal-article","created":{"date-parts":[[2026,3,24]],"date-time":"2026-03-24T08:18:04Z","timestamp":1774340284000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Arm\u2010Length\u2010Controlled CsPbBr\n                    <sub>3<\/sub>\n                    Nanocrystals for Tunable Optical and Assembly Behavior"],"prefix":"10.1002","volume":"38","author":[{"given":"Irina","family":"Skvortsova","sequence":"first","affiliation":[{"name":"Electron Microscopy for Materials Science (EMAT) &amp; NANOlight Center of Excellence University of Antwerp  Antwerp 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