This Ph.D. dissertation presents the design, synthesis, and application of a new class of dextran-based supramolecular hydrogels. Chemically modified dextrans bearing β-cyclodextrin (CD), adamantane (Ada), and benzophenone (Bzp) moieties were developed as modular building blocks. These hydrogels combine strong, reversible Ada/CD host-guest interactions - imparting dynamic, self-healing, and tunable viscoelastic properties - with photoinitiator-free UV curing enabled by Bzp/CD inclusion and subsequent covalent cross-linking.

Systematic investigation of gelation behavior revealed that hydrogel properties can be precisely tuned by varying solution concentration, anchor point ratio, polymer chain length, and composition. Polymer functionalization was achieved via azide–alkyne cycloaddition and nucleophilic acyl substitution and confirmed by NMR and FTIR. Hydrogel properties were systematically tuned through composition and molecular parameters, with rheology, UV curing, SAXS modeling, swelling, and microscopy revealing dynamic, self-healing networks with enhanced mechanical stability. 

In Paper I, the review article summarizes supramolecular hydrogels for tissue engineering, classifying them by interaction type and linking their dynamic properties to bioink performance.

In Paper II, UV-cured Bzp/CD hydrogels facilitated the co-immobilization of enzymes and electron mediators in bioelectrochemistry, achieving efficient mediated electron transfer with stable electrochemical performance. 

In Paper III, optimized formulations enabled good printability in 3D bioprinting. Cytotoxicity studies underscored the importance of supramolecular cross-linking in reducing the adverse effects of free polymer chains. Overall, this Ph.D. work establishes a flexible, biocompatible supramolecular hydrogel with broadly tunable properties, providing a foundation for future applications.