Self-healing bioinks with β-cyclodextrin–adamantine supramolecular interpenetrating polymer networks based on alginate and hyaluronic acid methacrylates for tissue engineering

Three-dimensional (3D) bioprinting has revolutionized the field of tissue engineering by enabling the fabrication of complex biological structures with high precision. The development of bioinks with enhanced mechanical, rheological, and biological properties is critical for advancing this technology. In this study, we designed biocompatible bioinks with self-healing capabilities using host-guest molecules modified onto two distinct polymeric networks. To achieve this, two different polymer chains were utilized: one was functionalized with a host molecule (β-cyclodextrin) and the other with a guest molecule (1-adamantane acetic acid). Alginate methacrylate (AlgMa) was synthesized and subsequently modified with the host molecule, while hyaluronic acid was methacrylated and then modified with the guest molecule. Consequently, host-guest interaction-based biominks with interpenetrating polymer network (IPN) structures were prepared, leading to the development of these advanced bioinks.The resulting interpenetrating polymer network (IPN) structures exhibited improved mechanical stability, as demonstrated by oscillation frequency sweep tests. Our bioinks demonstrated excellent shear-thinning behavior, facilitating printability and maintaining shape fidelity during and after the bioprinting process. These features make them highly suitable for use in tissue scaffold fabrication. By leveraging the unique properties of self-healing bioinks, we provide a significant contribution to the development of durable, functional materials for tissue engineering applications.