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Here, we introduce a programmable strategy to govern the 1D\u2010to\u20102D dimensional transition and structural width of DNA brick crystals by engineering their connecting interfaces. Using the number of interface connecting strands (\n                    <jats:italic>N<\/jats:italic>\n                    <jats:sub>x<\/jats:sub>\n                    ) as a quantitative design parameter, we discover a sharp dimensional threshold that is preserved across both honeycomb and square lattices. At\n                    <jats:italic>N<\/jats:italic>\n                    <jats:sub>x<\/jats:sub>\n                    \u00a0\u2264\u00a08, the assembly is strictly confined to one\u2010dimensional nanoribbons; whereas at\n                    <jats:italic>N<\/jats:italic>\n                    <jats:sub>x<\/jats:sub>\n                    \u00a0\u2265\u00a012, lateral coupling activates extended two\u2010dimensional arrays whose structural width increases monotonically with\n                    <jats:italic>N<\/jats:italic>\n                    <jats:sub>x<\/jats:sub>\n                    . Thermal and thermodynamic analyses reveal that this sharp threshold behavior is lattice\u2010independent and originates from the size\u2010dependent thermal stability of the laterally connected domains. Our work establishes interfacial connectivity as a predictive handle for the on\u2010demand engineering of self\u2010assembled nanostructures with programmable dimensionality and prescribed widths.\n                  <\/jats:p>","DOI":"10.1002\/anie.2278382","type":"journal-article","created":{"date-parts":[[2026,6,18]],"date-time":"2026-06-18T17:39:50Z","timestamp":1781804390000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Programming Dimensional Transitions in DNA Brick Crystals via Interfacial Connectivity"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0001-0908-2837","authenticated-orcid":false,"given":"Xin","family":"Huang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Synergistic Chem\u2010Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules Zhang Jiang 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Shanghai Jiao Tong University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunxiao","family":"Lin","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Synergistic Chem\u2010Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine Shanghai Jiao Tong University  Shanghai China"},{"name":"Zhangjiang Laboratory  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bochen","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Synergistic Chem\u2010Bio Synthesis School of Chemistry and Chemical Engineering New Cornerstone Science Laboratory Frontiers Science Center for Transformative Molecules Zhang Jiang Institute for Advanced Study and National Center for Translational Medicine Shanghai Jiao Tong 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