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Here, we compare Hyphantria cunea silk with Bombyx mori silk to examine how nanofibril-level load-transfer descriptors are associated with deformation when \u03b2-sheet fraction and axial orientation are comparable. Peptide profiling and single-fiber synchrotron infrared microspectroscopy show that H. cunea silk contains \u03b2-sheet-compatible sequence motifs and reaches \u03b2-sheet content and axial orientation comparable to those of B. mori silk. Despite this similarity, H. cunea silk exhibits a high-strength, near-linear tensile response, whereas B. mori silk follows a yielding\u2212extension\u2212hardening pathway. AFM-based fibrillar analysis and topology-constrained load-transfer modeling identify systematic differences in ex situ contour characteristics, effective coupling, and characteristic load-transfer descriptors that are consistent with the observed mechanical divergence. These results identify nanofibril coupling topology as a structural descriptor for programming silk fiber deformation beyond \u03b2-sheet order.<\/jats:p>","DOI":"10.1021\/acs.biomac.6c01384","type":"journal-article","created":{"date-parts":[[2026,9,11]],"date-time":"2026-09-11T17:02:01Z","timestamp":1789146121000},"page":"6764-6777","source":"Crossref","is-referenced-by-count":0,"title":["Topology-Constrained Load Transfer Reprograms Silk Fiber Deformation beyond \u03b2-Sheet Order"],"prefix":"10.1021","volume":"27","author":[{"given":"Yiyun","family":"Zhang","sequence":"first","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jing","family":"Ren","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0868-2934","authenticated-orcid":true,"given":"Jinrong","family":"Yao","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7706-4166","authenticated-orcid":true,"given":"Xin","family":"Chen","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ke","family":"Zheng","sequence":"additional","affiliation":[{"name":"Anhui Agricultural University , , , ,","place":["Hefei, Anhui, China, 230036"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5334-4008","authenticated-orcid":true,"given":"Zhengzhong","family":"Shao","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1156-0479","authenticated-orcid":true,"given":"Shengjie","family":"Ling","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200433"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,11]]},"reference":[{"issue":"5991","key":"2026101210570711900_cit1","doi-asserted-by":"publisher","first-page":"528","DOI":"10.1126\/science.1188936","article-title":"New Opportunities for an Ancient Material","volume":"329","author":"Omenetto","year":"2010","journal-title":"Science"},{"issue":"51","key":"2026101210570711900_cit2","doi-asserted-by":"publisher","first-page":"1903948","DOI":"10.1002\/smll.201903948","article-title":"Hierarchical Structure of Silk Materials Versus Mechanical Performance and Mesoscopic Engineering Principles","volume":"15","author":"Qiu","year":"2019","journal-title":"Small"},{"issue":"1","key":"2026101210570711900_cit3","doi-asserted-by":"publisher","first-page":"011313","DOI":"10.1063\/1.5091442","article-title":"Engineering Silk Materials: From Natural Spinning to Artificial Processing","volume":"7","author":"Guo","year":"2020","journal-title":"Appl. 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