Engineering nanocomposite hydrogels using dynamic bonds

Nanocomposite (NC) hydrogels are promising biomaterials that possess versatile properties and functions for biomedical applications such as drug delivery, biosensor development, imaging and tissue engineering. Different strategies and chemistries have been utilized to define the structure and properties of NC hydrogels. In this review, we discuss NC hydrogels synthesized using dynamic bonds, including dynamic covalent bonds (e.g., Schiff base and boronate ester bond) and non-covalent bonds (e.g., hydrogen bonds and metal-ligand coordination). Dynamic bonds can reversibly break and reform to provide self-healing properties to NC hydrogels as well as be influenced by external factors to allow NC hydrogels with stimulus-responsiveness. The presence of dynamic bonds in NC hydrogels can occur at the polymer-polymer or polymer-particle interfaces, which also determines whether the particles act as fillers or crosslinkers in hydrogels. Several representative examples of NC hydrogels fabricated using dynamic bonds are discussed here, focusing on their design, preparation, properties, applications and future prospects. This review provides an overview of the current progress in NC hydrogel development using dynamic bonds, summarizing the material design, fabrication approaches, unique performance and promising biomedical applications. The presence of both nanoparticles and dynamic bonds in hydrogels shows a combined or synergistic effect to provide hydrogels with dynamic features, definable properties, multi-functionality and stimulus-responsiveness for advanced applications. We believe that this review will be of interest to the hydrogel community and inspire researchers to develop next-generation hydrogels.