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Extending this concept to organic 2D crystals has been hindered by weak, non-directional interlayer interactions that frustrate lattice registry. Here we introduce a bottom-up strategy for programmable lattice engineering in organic van der Waals heterostructures of 2D polymers. Sequential on-water-surface assembly enables layer-by-layer stacking of chemically distinct 2D polymers with defined lattice registry, stacking sequence and thickness, yielding both lattice-matched and controlled lattice-mismatched heterostructures. Structural characterization reveals commensurate epitaxy in lattice-matched and small-mismatched systems, whereas large-mismatch interfaces exhibit moir\u00e9 features and strain-relief distortions. Ultrafast spectroscopy demonstrates efficient interfacial charge separation and first-principles calculations reveal built-in electric fields and interfacial potential steps arising from interfacial dipole alignment. Devices exhibit diode-like rectification ratios exceeding 10\n                    <jats:sup>7<\/jats:sup>\n                    that systematically decrease with increasing lattice mismatch, establishing organic 2D polymer van der Waals heterostructures as a lattice-engineered platform for (opto)electronic and quantum phenomena.\n                  <\/jats:p>","DOI":"10.1038\/s41586-026-11074-6","type":"journal-article","created":{"date-parts":[[2026,9,23]],"date-time":"2026-09-23T15:05:57Z","timestamp":1790175957000},"page":"388-397","update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Organic two-dimensional van der Waals heterostructures"],"prefix":"10.1038","volume":"658","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1573-7008","authenticated-orcid":false,"given":"Anupam","family":"Prasoon","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9678-6356","authenticated-orcid":false,"given":"Nguyen Ngan","family":"Nguyen","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8487-0972","authenticated-orcid":false,"given":"Mike","family":"Hambsch","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Puja","family":"Singhvi","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sophia","family":"Terres","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zijie","family":"Xiao","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Naveen","family":"Goyal","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoyuan","family":"Qi","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David","family":"M\u00fccke","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1709-4384","authenticated-orcid":false,"given":"Florian","family":"Auras","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhiyong","family":"Wang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3953-5208","authenticated-orcid":false,"given":"Sein","family":"Chung","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3016-9523","authenticated-orcid":false,"given":"Miroslav","family":"Polo\u017eij","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0940-3984","authenticated-orcid":false,"given":"Hai I.","family":"Wang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0321-3629","authenticated-orcid":false,"given":"Kilwon","family":"Cho","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0582-4044","authenticated-orcid":false,"given":"Ute","family":"Kaiser","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9213-2777","authenticated-orcid":false,"given":"Alexey","family":"Chernikov","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6851-8453","authenticated-orcid":false,"given":"Mischa","family":"Bonn","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0268-519X","authenticated-orcid":false,"given":"Stefan C. 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