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However, fields such as biomaterials require wavelength outside the harsh UV regime to prevent photodamage, typically requiring chromophores with extended \u03c0\u2010conjugation that suffer from poor water solubility. Herein, we demonstrate how cyclodextrins can be used as auxiliary agents to not only solubilize such chromophores, but even to preorganize them in a 2\u2009:\u20092 host\u2010guest inclusion complex to facilitate photodimerization. We apply our concept to styrylpyrene\u2010end\u2010functionalized star\u2010shaped polyethylene glycols (sPEGs). We initially unravel details of the host\u2010guest inclusion complex using spectroscopy and mass spectrometry to give clear evidence of a 2\u2009:\u20092 complex formation. Subsequently, we show that the resultant supramolecularly linked hydrogels conform to theories of supramolecular quasi\u2010ideal model networks, and derive details on their association dynamics using in\u2010depth rheological measurements and kinetic models. By comparing sPEGs of different arm length, we further elucidate the model network topology and the accessible mechanical property space. The photo\u2010mediated dimerization proceeds smoothly, allowing to transform the supramolecular model networks into covalent ones. We submit that our strategy opens avenues for executing hydrophobic photochemistry in aqueous environments with enhanced control over reactivity, hydrogel topology or programmable mechanical properties.<\/jats:p>","DOI":"10.1002\/anie.202405582","type":"journal-article","created":{"date-parts":[[2024,4,19]],"date-time":"2024-04-19T12:19:55Z","timestamp":1713529195000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Cyclodextrin \u2018Chaperones\u2019 Enable Quasi\u2010Ideal Supramolecular Network Formation and Enhanced Photodimerization of Hydrophobic, Red\u2010shifted Photoswitches in Water"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-9747-1910","authenticated-orcid":false,"given":"Daniel","family":"Hoenders","sequence":"first","affiliation":[{"name":"Life-Like Materials and Systems Lab Department of Chemistry University of Mainz  Duesbergweg\u200510\u201314 55128 Mainz Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Simon","family":"Ludwanowski","sequence":"additional","affiliation":[{"name":"Life-Like Materials and Systems Lab Department of Chemistry University of Mainz  Duesbergweg\u200510\u201314 55128 Mainz Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6745-0570","authenticated-orcid":false,"given":"Christopher","family":"Barner\u2010Kowollik","sequence":"additional","affiliation":[{"name":"School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology (QUT)  2 George Street, 4000 Brisbane, QLD Australia"},{"name":"Institute of Nanotechnology (INT) Karlsruhe Institute of Technology (KIT)  Hermann-von-Helmholtz-Platz\u20051 76344 Eggenstein-Leopoldshafen Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2170-3306","authenticated-orcid":false,"given":"Andreas","family":"Walther","sequence":"additional","affiliation":[{"name":"Life-Like Materials and Systems Lab Department of Chemistry University of Mainz  Duesbergweg\u200510\u201314 55128 Mainz Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2024,5,24]]},"reference":[{"key":"e_1_2_8_1_1","unstructured":"\u00a0"},{"key":"e_1_2_8_2_2","doi-asserted-by":"publisher","DOI":"10.1038\/natrevmats.2017.87"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201807333"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.matt.2021.03.021"},{"key":"e_1_2_8_5_2","doi-asserted-by":"publisher","DOI":"10.1002\/marc.202100703"},{"key":"e_1_2_8_6_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.actbio.2021.10.003"},{"key":"e_1_2_8_7_1","unstructured":"\u00a0"},{"key":"e_1_2_8_8_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c09419"},{"key":"e_1_2_8_9_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-022-30002-6"},{"key":"e_1_2_8_10_2","doi-asserted-by":"publisher","DOI":"10.1039\/D1SC06154B"},{"key":"e_1_2_8_11_2","author":"Eren T. 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