Schiff base, an important family of reaction in click chemistry, has received significant attention in the formation of self-healing hydrogels in recent years. Schiff base reversibly reacts even in mild conditions, which allows hydrogels with self-healing ability to recover their structures and functions after damages. Moreover, pH-sensitivity of the Schiff base offers the hydrogels response to biologically relevant stimuli. Different types of Schiff base can provide the hydrogels with tunable mechanical properties and chemical stabilities. In this review, we summarized the design and preparation of hydrogels based on various types of Schiff base linkages, as well as the biomedical applications of hydrogels in drug delivery, tissue regeneration, wound healing, tissue adhesives, bioprinting, and biosensors.

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Hydrogels, which are crosslinked polymer networks with high water contents and rheological solid-like properties, are attractive materials for biomedical applications. Self-healing hydrogels are particularly interesting because of their abilities to repair the structural damages and recover the original functions, similar to the healing of organism tissues. In addition, self-healing hydrogels with shear-thinning properties can be potentially used as the vehicles for drug/cell delivery or the bioinks for 3D printing by reversible sol-gel transitions. Therefore, self-healing hydrogels as biomedical materials have received a rapidly growing attention in recent years. In this paper, synthesis methods and repair mechanisms of self-healing hydrogels are reviewed. The biomedical applications of self-healing hydrogels are also described, with a focus on the potential therapeutic applications verified through in vivo experiments. The trends indicate that self-healing hydrogels with automatically reversible crosslinks may be further designed and developed for more advanced biomedical applications in the future.