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Although layer-transfer methods are effective for device prototyping, managing crack formation during this process is challenging. In this study, we investigate the fracture mechanics of bilayer-type organic semiconductor (OSC) films as a model for developing a crack-suppressed transfer methodology. We find that crack formation is strongly dependent on film thickness and is suppressed when the film is reduced to a single molecular bilayer (SMB) thickness. The observed crack directionality in thick films is clearly correlated with the crystallographic orientation. These fracture behaviors can be qualitatively explained by combining a macroscopic elasticity model with calculations of intermolecular interaction energies. Based on this understanding, we successfully fabricate highly ordered multilayered artificial lattices through sequential SMB transfers. Furthermore, by expanding the \u03c0-electron core to tune intermolecular interactions, we achieve the direct patterning of OSC films, even on lyophobic substrates, providing a suitable interface for organic thin-film transistors (OTFTs). OTFTs incorporating crack-suppressed SMBs exhibit sharp on\/off switching with a subthreshold swing of less than 150 mV dec\u20131 and a relatively high device mobility exceeding 5 cm2 V\u20131 s\u20131. These findings pave the way for molecular layer engineering for surface tailoring and organic device manufacturing.<\/jats:p>","DOI":"10.1021\/acsami.6c12628","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T16:11:06Z","timestamp":1788451866000},"page":"49581-49589","source":"Crossref","is-referenced-by-count":0,"title":["Mechanics-Guided Layer-by-Layer Transfer of Molecular Bilayer Semiconductors"],"prefix":"10.1021","volume":"18","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-0055-3006","authenticated-orcid":true,"given":"Shunto","family":"Arai","sequence":"first","affiliation":[{"name":"National Institute for Materials Science (NIMS) , 1-1 Namiki , , ,","place":["Tsukuba, Ibaraki, Japan, 305-0044"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mariko","family":"Shimokawa","sequence":"additional","affiliation":[{"name":"National Institute for Materials Science (NIMS) , 1-1 Namiki , , ,","place":["Tsukuba, Ibaraki, Japan, 305-0044"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takayuki","family":"Harada","sequence":"additional","affiliation":[{"name":"National Institute for Materials Science (NIMS) , 1-1 Namiki , , ,","place":["Tsukuba, Ibaraki, Japan, 305-0044"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9227-8207","authenticated-orcid":true,"given":"Toshiki","family":"Higashino","sequence":"additional","affiliation":[{"name":"National Institute of Advanced Industrial Science and Technology (AIST) , 1-1-1 Higashi , , ,","place":["Tsukuba, Ibaraki, Japan, 305-8565"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,2]]},"reference":[{"key":"2026091615065175700_cit1","doi-asserted-by":"publisher","first-page":"706","DOI":"10.1038\/nature07719","article-title":"Large-scale Pattern Growth of Graphene Films for Stretchable Transparent Electrodes","volume":"457","author":"Kim","year":"2009","journal-title":"Nature"},{"key":"2026091615065175700_cit2","doi-asserted-by":"publisher","DOI":"10.1088\/1361-6528\/aabd90","article-title":"Minimizing residues and strain in 2D materials transferred from PDMS","volume":"29","author":"Jain","year":"2018","journal-title":"Nanotechnology"},{"issue":"5806","key":"2026091615065175700_cit3","doi-asserted-by":"publisher","first-page":"1754","DOI":"10.1126\/science.1132394","article-title":"Heterogeneous three-dimensional electronics by use of printed semiconductor nanomaterials","volume":"314","author":"Ahn","year":"2006","journal-title":"Science"},{"key":"2026091615065175700_cit4","doi-asserted-by":"publisher","first-page":"275","DOI":"10.1080\/14686996.2022.2062576","article-title":"Science of 2.5 dimensional materials: paradigm shift of materials science toward future social innovation","volume":"23","author":"Ago","year":"2022","journal-title":"Sci. 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