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The growing body of evidence that cell behavior depends upon hydrogel stress relaxation creates a high demand for hydrogels with tissue\u2010like viscoelastic properties. Here, a unique platform of synthetic polyethylene glycol (PEG) hydrogels in which star\u2010shaped PEG molecules are conjugated with alendronate and\/or RGD peptides, attaining modifiable degradability as well as flexible cell adhesion, is created. Novel reversible ionic interactions between alendronate and calcium phosphate nanoparticles, leading to versatile viscoelastic properties with varying initial elastic modulus and stress relaxation time, are identified. This new crosslinking mechanism provides shear\u2010thinning properties resulting in differential cellular responses between cancer cells and stem cells. The novel hydrogel system is an improved design to the other ionic crosslink platforms and opens new avenues for the development of pathologically relevant cancer models, as well as minimally invasive approaches for cell delivery for potential regenerative therapies.<\/jats:p>","DOI":"10.1002\/adhm.202400472","type":"journal-article","created":{"date-parts":[[2024,5,29]],"date-time":"2024-05-29T10:23:52Z","timestamp":1716978232000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Injectable PEG Hydrogels with Tissue\u2010Like Viscoelasticity Formed through Reversible Alendronate\u2013Calcium Phosphate Crosslinking for Cell\u2013Material Interactions"],"prefix":"10.1002","volume":"13","author":[{"given":"Hongqiang","family":"Yu","sequence":"first","affiliation":[{"name":"Centre for Craniofacial and Regenerative Biology King's College London  London UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziqian","family":"Yan","sequence":"additional","affiliation":[{"name":"Centre for Craniofacial and Regenerative Biology King's College London  London UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cecile A.","family":"Dreiss","sequence":"additional","affiliation":[{"name":"Institute of Pharmaceutical Science King's College London  London SE1 9NH UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gustavo G.","family":"Gaitano","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Navarra  Pamplona 31080 Spain"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"James A.","family":"Jarvis","sequence":"additional","affiliation":[{"name":"Randall Division of Cell and Molecular Biophysics and NMR Facility Centre for Biomolecular Spectroscopy King's College London  London SE1 1UL UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Eileen","family":"Gentleman","sequence":"additional","affiliation":[{"name":"Centre for Craniofacial and Regenerative Biology King's College London  London UK"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ricardo M. 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