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Multivalent binding is a powerful strategy, but the irrational spatial distribution of the functional moieties may reduce the probe performance. Here, we constructed a Janus DNA triangular prism nanostructure (3Zy1\u2010JTP\u20103) for sensitive detection and specific isolation of tumor cells. Benefiting from spatial features of the triangular prism, the fluorescence intensity induced by 3Zy1\u2010JTP\u20103 was almost 4 times that of the monovalent structure. Moreover, the DNA triangular prisms were connected to form hand\u2010in\u2010hand multivalent DNA triangular prism structures (Zy1\u2010MTP), in which the fluorescence intensity and affinity were increased to 9\u2010fold and 10\u2010fold of 3Zy1\u2010JTP\u20103, respectively. Furthermore, 3Zy1\u2010JTP\u20103 and Zy1\u2010MTP were combined with magnetic beads, and the latter showed higher capture efficiency (&gt;90\u2009%) in whole blood. This work provides a new strategy for the efficient capture of rare cells in complex biological samples.<\/jats:p>","DOI":"10.1002\/anie.202411382","type":"journal-article","created":{"date-parts":[[2024,10,15]],"date-time":"2024-10-15T11:13:56Z","timestamp":1728990836000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":16,"title":["Spatially Controlled DNA Frameworks for Sensitive Detection and Specific Isolation of Tumor Cells"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-4257-4304","authenticated-orcid":false,"given":"Lei","family":"Luo","sequence":"first","affiliation":[{"name":"State key Laboratory of Chemo\/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Key Laboratory for Bio-Nanotechnology and Molecular Engineering of Hunan Province Hunan University  Changsha 410082 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