{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,4,23]],"date-time":"2026-04-23T09:53:33Z","timestamp":1776938013181,"version":"3.51.4"},"reference-count":73,"publisher":"MDPI AG","issue":"4","license":[{"start":{"date-parts":[[2026,4,10]],"date-time":"2026-04-10T00:00:00Z","timestamp":1775779200000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":["Gels"],"abstract":"<jats:p>Hybrid supramolecular\u2013nanocomposite hydrogels based on polyethylene glycol (PEG), \u03b2-cyclodextrin\u2013adamantane host\u2013guest interactions, and silica nanoparticles represent an important class of hierarchical soft materials with tunable viscoelastic and transport properties. This review critically analyzes recent progress in cyclodextrin\u2013silica hybrid PEG hydrogels, focusing on the mechanistic coupling between stiffness, stress relaxation, and molecular transport arising from the interplay between reversible supramolecular crosslinks and nanoparticle-induced confinement effects. Particular attention is given to how host\u2013guest exchange kinetics regulate dynamic bond rearrangement and affinity-mediated retention of hydrophobic cargo, while silica nanoparticles enhance mechanical reinforcement and modify diffusion pathways through tortuosity and interfacial polymer\u2013particle interactions. The analysis highlights how nanoparticle size, loading level, and surface functionalization influence relaxation spectra and network topology, as well as how environmental stimuli may affect supramolecular bond stability and overall material performance. Comparison with alternative inorganic fillers and mesoporous silica architectures further clarifies the specific advantages of silica in achieving balanced mechanical stability and controlled transport behavior. Overall, current evidence indicates that hybrid CD\u2013silica networks enable partial decoupling of stiffness, relaxation dynamics, and diffusion, although complete independence remains constrained by fundamental polymer physics relationships. These insights support the development of predictive structure\u2013property frameworks for advanced biomedical and controlled release applications.<\/jats:p>","DOI":"10.3390\/gels12040323","type":"journal-article","created":{"date-parts":[[2026,4,10]],"date-time":"2026-04-10T10:20:16Z","timestamp":1775816416000},"page":"323","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Cyclodextrin\u2013Silica Hybrid PEG Hydrogels: Mechanistic Coupling Between Stiffness, Relaxation, and Molecular Transport"],"prefix":"10.3390","volume":"12","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8671-0705","authenticated-orcid":false,"given":"Anca Daniela","family":"Raiciu","sequence":"first","affiliation":[{"name":"Department of Pharmacognosy, Phytochemistry, and Phytotherapy, Faculty of Pharmacy, Titu Maiorescu University, Gh. \u015eincai Street No. 16, District 4, 040314 Bucharest, Romania"},{"name":"PLANTA ROMANICA Association, George Enescu Street No. 27-29, District 1, 010303 Bucharest, Romania"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7254-7991","authenticated-orcid":false,"given":"Amalia","family":"Stefaniu","sequence":"additional","affiliation":[{"name":"National Institute for Chemical Pharmaceutical Research and Development, ICCF, 12 Vitan Av. District 3, 031299 Bucharest, Romania"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"1968","published-online":{"date-parts":[[2026,4,10]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","unstructured":"Voros-Horv\u00e1th, B., Salem, A., Kov\u00e1cs, B., Sz\u00e9chenyi, A., and P\u00e1l, S. (2024). Systematic Study of Reaction Conditions for Size-Controlled Synthesis of Silica Nanoparticles. Nanomaterials, 14.","DOI":"10.20944\/preprints202409.0025.v1"},{"key":"ref_2","doi-asserted-by":"crossref","unstructured":"Liu, Y., He, W., Zhang, Z., and Lee, B.P. (2018). Recent Developments in Tough Hydrogels for Biomedical Applications. Gels, 4.","DOI":"10.3390\/gels4020046"},{"key":"ref_3","doi-asserted-by":"crossref","first-page":"71","DOI":"10.1146\/annurev-matsci-070218-010015","article-title":"Opportunities and Challenges for Machine Learning in Materials Science","volume":"50","author":"Morgan","year":"2020","journal-title":"Annu. Rev. Mater. 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