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Owing to their reversible physical crosslinking and versatile design strategies, hydrogen bonds can endow linear PDMS with a broader spectrum of performance possibilities. However, the construction of hydrogen-bonded PDMS elastomers that simultaneously achieve both outstanding mechanical performance and reversible interfacial adhesion remains a significant challenge. Herein, we report the first design and synthesis of linear PDMS elastomers dynamically crosslinked by dense multiple hydrogen-bonding arrays derived from oxalyl dihydrazide (ODH). A series of silicone poly(urea oxalyl dihydrazide) (SPUOH) elastomers were synthesized via a one-pot method by tailoring the molecular weight of the \u03b1, \u03c9-bis (aminopropyl) polydimethylsiloxanes (A-PDMS) and the ODH loading. The synergistic interplay of strong ODH-based hydrogen bonds and weak urea-based hydrogen bonds enables tunable mechanical properties: SPUOH-3k-0.33 achieves a tensile strength of 5.15 MPa, an elongation at break of \u223c1200%, and a toughness of 39.8 MJ m\u20133, substantially surpassing reported linear PDMS elastomers. Rheological and AFM analyses reveal that hydrogen-bond ordering governs thermal resistance and microphase separation, with high ODH loading inducing a phase inversion. Benefiting from thermally reversible hydrogen bonds, SPUOH-3k-0.33 exhibits a lap shear strength of 2.72 MPa on polyamide and maintains performance over 20 cycles. A prototype flexible sensor demonstrates a gauge factor of 4.6 with reliable motion monitoring. This work establishes ODH-based hydrogen-bonding arrays as a versatile platform for high-performance, sustainable, and adhesively integrable PDMS substrates for next-generation flexible electronics.<\/jats:p>","DOI":"10.1021\/acsami.6c15060","type":"journal-article","created":{"date-parts":[[2026,10,17]],"date-time":"2026-10-17T15:06:21Z","timestamp":1792249581000},"source":"Crossref","is-referenced-by-count":0,"title":["High-Performance PDMS Elastomers Constructed via Oxalyl Dihydrazide for Thermoreversible Bonding in Flexible Electronics"],"prefix":"10.1021","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-0897-1295","authenticated-orcid":true,"given":"Chenxi","family":"Lin","sequence":"first","affiliation":[{"name":"South China University of Technology (SCUT) , , ,","place":["Guangzhou, P. R. China, 510640"]},{"name":"South China University of Technology (SCUT) , , ,","place":["Guangzhou, P. R. China, 510640"]},{"name":"South China University of Technology (SCUT) , , ,","place":["Guangzhou, P. R. China, 510640"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8857-3879","authenticated-orcid":true,"given":"Jianhui","family":"Xia","sequence":"additional","affiliation":[{"name":"South China University of Technology (SCUT) , , ,","place":["Guangzhou, P. R. China, 510640"]},{"name":"South China University of Technology (SCUT) , , ,","place":["Guangzhou, P. R. China, 510640"]},{"name":"South China University of Technology (SCUT) , , ,","place":["Guangzhou, P. R. China, 510640"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,19]]},"reference":[{"issue":"3","key":"2026101711024562900_cit1","doi-asserted-by":"publisher","first-page":"4568","DOI":"10.1021\/acsami.5c16200","article-title":"Bioinspired Flexible Tactile Sensors for Smart Soft Robotics","volume":"18","author":"Wang","year":"2026","journal-title":"ACS Appl. Mater. 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