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Asymmetric block extension of one arm for star\u2010shaped poly(ethylene glycol) [PEG<jats:sub>26<\/jats:sub>\u2010SH]<jats:sub>4<\/jats:sub> using short segments of polyampholytic poly(dehydroalanine) (PDha) is herein demonstrated while maintaining the functional thiol end groups for network formation. For subsequent hydrogel synthesis with up to 10\u00a0wt.% PDha a straightforward and biocompatible photoinitiated thiol\u2010ene click reaction is exploited. The investigation of the swelling properties of the hydrogel revealed responsive behavior toward ionic strength and variations in pH value. Moreover, the reversible adsorption of the model dyes methylene blue (MB) and acid orange 7 (AO7) is investigated by UV\u2013vis measurements and the procedure can be successfully transferred to the adsorption of the adhesion peptide RGDS resulting in an uptake of 1.5 wt% RGDS with regard to the dry weight of the hydrogel.<\/jats:p>","DOI":"10.1002\/mabi.202300230","type":"journal-article","created":{"date-parts":[[2023,8,12]],"date-time":"2023-08-12T17:03:20Z","timestamp":1691859800000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Asymmetric Block Extension of Star\u2010Shaped [PEG\u2010SH]<sub>4<\/sub> \u2013 toward Poly(dehydroalanine)\u2010Functionalized PEG Hydrogels for Catch and Release of Charged Guest Molecules"],"prefix":"10.1002","volume":"24","author":[{"given":"Kathrin","family":"Kowalczuk","sequence":"first","affiliation":[{"name":"Institute of Organic Chemistry and Macromolecular Chemistry (IOMC) 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