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Herein, a simple method is reported to prepare photodegradable double\u2010network (DN) hydrogels that exhibit high stretchability, toughness, and biocompatibility. Hydrophilic <jats:italic>ortho<\/jats:italic>\u2010nitrobenzyl (ONB) crosslinkers incorporating different poly(ethylene glycol) (PEG) backbones (600, 1000, and 2000\u00a0g\u00a0mol<jats:sup>\u22121<\/jats:sup>) are synthesized. These photodegradable DN hydrogels are prepared by the irreversible crosslinking of chains by using such ONB crosslinkers, and the reversible ionic crosslinking between sodium alginate and divalent cations (Ca<jats:sup>2+<\/jats:sup>). Remarkable mechanical properties are obtained by combining ionic and covalent crosslinking and their synergistic effect, and by reducing the length of the PEG backbone. The rapid on\u2010demand degradation of these hydrogels is also demonstrated by using cytocompatible light wavelength (<jats:italic>\u03bb<\/jats:italic>\u00a0=\u00a0365\u00a0nm) that degrades the photosensitive ONB units. The authors have successfully used these hydrogels as skin\u2010worn sensors for monitoring human respiration and physical activities. A combination of excellent mechanical properties, facile fabrication, and on\u2010demand degradation holds promise for their application as the next generation of substrates or active sensors eco\u2010friendly for bioelectronics, biosensors, wearable computing, and stretchable electronics.<\/jats:p>","DOI":"10.1002\/adhm.202300918","type":"journal-article","created":{"date-parts":[[2023,5,3]],"date-time":"2023-05-03T11:29:09Z","timestamp":1683113349000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Facile Synthesis of Highly Stretchable, Tough, and Photodegradable Hydrogels"],"prefix":"10.1002","volume":"12","author":[{"given":"Rita G.","family":"Fonseca","sequence":"first","affiliation":[{"name":"CEMMPRE \u2013 Department of Chemical Engineering University of Coimbra  Coimbra 3030\u2013790 Portugal"}]},{"given":"Aline","family":"Kuster","sequence":"additional","affiliation":[{"name":"CEMMPRE \u2013 Department of Chemical Engineering University of Coimbra  Coimbra 3030\u2013790 Portugal"}]},{"given":"Pedro P.","family":"Fernandes","sequence":"additional","affiliation":[{"name":"Soft and Printed Microelectronics Lab Department of Electrical Engineering University of Coimbra  Coimbra 3030\u2013194 Portugal"}]},{"given":"Mahmoud","family":"Tavakoli","sequence":"additional","affiliation":[{"name":"Soft and Printed Microelectronics Lab Department of Electrical Engineering University of Coimbra  Coimbra 3030\u2013194 Portugal"}]},{"given":"Patr\u00edcia","family":"Pereira","sequence":"additional","affiliation":[{"name":"CEMMPRE \u2013 Department of Chemical Engineering University of Coimbra  Coimbra 3030\u2013790 Portugal"},{"name":"IPN \u2013 Instituto Pedro Nunes Associa\u00e7\u00e3o para a Inova\u00e7\u00e3o e Desenvolvimento em Ci\u00eancia e Tecnologia  Rua Pedro Nunes Coimbra 3030\u2013199 Portugal"}]},{"given":"Jos\u00e9 R.","family":"Fernandes","sequence":"additional","affiliation":[{"name":"Chemical Centre \u2013 Vila Real (CQVR) Physics Department School of Science and Technology University of Tr\u00e1s\u2010os\u2010Montes e Alto Douro  Vila Real 5000\u2013801 Portugal"}]},{"given":"Francesco","family":"De Bon","sequence":"additional","affiliation":[{"name":"CEMMPRE \u2013 Department of Chemical Engineering University of Coimbra  Coimbra 3030\u2013790 Portugal"}]},{"given":"Arm\u00e9nio C.","family":"Serra","sequence":"additional","affiliation":[{"name":"CEMMPRE \u2013 Department of Chemical Engineering University of Coimbra  Coimbra 3030\u2013790 Portugal"}]},{"given":"Ana C.","family":"Fonseca","sequence":"additional","affiliation":[{"name":"CEMMPRE \u2013 Department of Chemical Engineering University of Coimbra  Coimbra 3030\u2013790 Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9351-1704","authenticated-orcid":false,"given":"Jorge F. 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