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However, fabricating single\u2010crystal architectures featuring numerous shells with intricate distribution patterns remains challenging. In this study, we employed DNA nanotechnology to construct microscale multilayer core\u2013shell DNA origami crystals. The internal layers exhibit tunable properties, including size, quantity, self\u2010similarity, and morphology. The shell size can be regulated from 700 to 1800 \u00b5m\n                    <jats:sup>3<\/jats:sup>\n                    , and the layer quantity can be extended to five. We also fabricated eight distinct crystals exhibiting non\u2010self\u2010similarity and two types of heteromorphic core\u2013shell crystals. Each layer has operational independence, allowing the customized capture of nanomaterials and implementation of compartmentalized reactions. These multilayer core\u2013shell crystals have potential for serving as compartmentalization templates for functional units, which may provide possibilities for simulating cell work or constructing artificial organelles.\n                  <\/jats:p>","DOI":"10.1002\/adma.74163","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T11:14:01Z","timestamp":1784286841000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Hierarchical Assembly of Multilayer Core\u2013Shell DNA Origami Crystals"],"prefix":"10.1002","volume":"38","author":[{"given":"Yifan","family":"Yu","sequence":"first","affiliation":[{"name":"Department of Orthopedic Surgery Nanjing Drum Tower Hospital College of Engineering and Applied Sciences State Key Laboratory of Analytical Chemistry for Life Science National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional Materials Chemistry and Biomedicine Innovation Center Collaborative\u00a0Innovation\u00a0Center\u00a0of\u00a0Advanced\u00a0Microstructures Nanjing University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hang","family":"Xu","sequence":"additional","affiliation":[{"name":"Department of Orthopedic Surgery Nanjing Drum Tower Hospital College of Engineering and Applied Sciences State Key Laboratory of Analytical Chemistry for Life Science National Laboratory of Solid State Microstructures Jiangsu Key Laboratory of Artificial Functional Materials Chemistry and Biomedicine Innovation Center Collaborative\u00a0Innovation\u00a0Center\u00a0of\u00a0Advanced\u00a0Microstructures Nanjing University  Nanjing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuehui","family":"Yan","sequence":"additional","affiliation":[{"name":"Department of Orthopedic Surgery Nanjing Drum Tower Hospital College of Engineering and Applied Sciences State Key Laboratory of 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