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This work aims to improve the mechanical properties of starch-based hydrogels using a double-network (DN) strategy. The single network (SN) starch hydrogel was first prepared using glutaraldehyde as a crosslinker. The compressive properties of the SN hydrogels were influenced by both crosslinker content and crosslinking time. The SN starch hydrogel possessing the best mechanical properties was then fabricated into DN hydrogels. Poly(vinyl alcohol) (PVA) and borax were used as a secondary polymer and a crosslinker, respectively. The PVA–borax complexation partly enhanced the DN hydrogel's compressive modulus by 30% and its toughness by 39%. DN hydrogels were found to have denser microstructures than SN hydrogels. To be specific, their walls thickened and grew more continuous while their pores shrank. The increased crosslinking density resulted in changes to the microstructure, which were well correlated with their porosity and water uptake capacity. An in vitro cytotoxicity test of the DN hydrogels revealed that they were non-toxic to chondrocytes. This work demonstrated that double networking is a simple but effective strategy for improving mechanical properties of starch-based hydrogels without sacrificing their biocompatibility. This approach can be used to tailor hydrogel properties to fulfill requirements for biomedical applications, such as tissue engineering and other related fields. [ABSTRACT FROM AUTHOR]

Attaching hydrogels to soft internal tissues is crucial for the development of various biomedical devices. Tough sticky hydrogel patches present high adhesion, yet with lack of injectability and the need for treatment of contacting surface. On the contrary, injectable and photo‐curable hydrogels are highly attractive owing to their ease of use, flexibility of filling any shape, and their minimally invasive character, compared to their conventional preformed counterparts. Despite recent advances in material developments, a hydrogel that exhibits both proper injectability and sufficient intrinsic adhesion is yet to be demonstrated. Herein, a paradigm shift is proposed toward the design of intrinsically adhesive networks for injectable and photo‐curable hydrogels. The bioinspired design strategy not only provides strong adhesive contact, but also results in a wide window of physicochemical properties. The adhesive networks are based on a family of polymeric backbones where chains are modified to be intrinsically adhesive to host tissue and simultaneously form a hydrogel network via a hybrid cross‐linking mechanism. With this strategy, adhesion is achieved through a controlled synergy between the interfacial chemistry and bulk mechanical properties. The functionalities of the bioadhesives are demonstrated for various applications, such as tissue adhesives, surgical sealants, or injectable scaffolds. [ABSTRACT FROM AUTHOR]