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These materials are commonly fabricated through confined self\u2010assembly of block copolymers (BCPs) in evaporative emulsions, which can proceed by either microphase separation or organized spontaneous emulsification (OSE) to yield lamellar or porous structures with complementary optical responses. In this study, we show that amphiphilic dendronized brush block copolymers (den\u2010BBCPs) exhibit mechanism\u2010selective self\u2010assembly governed by the volume fraction (\n                    <jats:italic>f)<\/jats:italic>\n                    of hydrophilic segment. At\n                    <jats:italic>f<\/jats:italic>\n                    &lt; 50%, den\u2010BBCPs follow the OSE pathway, generating photonic microspheres with short\u2010range\u2010ordered porous structures and angle\u2010independent structural colors. In contrast, at\n                    <jats:italic>f<\/jats:italic>\n                    &gt; 50%, microphase separation dominates, producing concentric lamellar microspheres with strong specular reflections. This pathway transition arises from the rigid dendronized architecture: increasing the volume fraction of hydrophilic segment amplifies intermolecular repulsions at the highly curved water\u2010in\u2010oil nanodroplet interface, destabilizing interfacial association and redirecting assembly toward microphase separation. This work establishes architectural engineering of den\u2010BBCPs as a powerful strategy for programming self\u2010assembly pathways and creating polymeric photonic pigments with diverse structures and optical properties.\n                  <\/jats:p>","DOI":"10.1002\/anie.3308853","type":"journal-article","created":{"date-parts":[[2026,8,25]],"date-time":"2026-08-25T11:24:24Z","timestamp":1787657064000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mechanism\u2010Selective Self\u2010Assembly of Amphiphilic Dendronized Brush Block Copolymers Into Lamellar and Porous Photonic Pigments"],"prefix":"10.1002","volume":"65","author":[{"given":"Mohan","family":"Zheng","sequence":"first","affiliation":[{"name":"Tianjin Key Laboratory of Composite and Functional Materials School of Materials Science and Engineering Tianjin University  Tianjin 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