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Supramolecular hydrogels play a prominent role in contemporary research of hydrophilic polymers. Especially, hydrogels based on α-cyclodextrin/poly(ethylene glycol) (α-CD/PEG) complexation and crystal formation are studied frequently. Here, the effect of double hydrophilic block copolymers (DHBCs) on α-CD/PEG hydrogel properties is investigated. Therefore, a novel DHBC, namely poly( N -vinylpyrrolidone)- b -poly(oligo ethylene glycol methacrylate) (PVP- b -POEGMA), was synthesized via a combination of reversible deactivation radical polymerization and modular conjugation methods. In the next step, hydrogel formation was studied after α-CD addition. Interestingly, DHBC-based hydrogels showed a significant response to thermal history. Heating of the gels to different temperatures led to different mechanical properties after cooling to ambient temperature, i.e., gels with mechanical properties similar to the initial gels or weak flowing gels were obtained. Thus, the hydrogels showed thermoadaptive behavior, which might be an interesting property for future applications in sensing.

Thermoadaptive Supramolecular α-Cyclodextrin Crystallization-Based Hydrogels via Double Hydrophilic Block Copolymer Templating