Regenerated silk fibroin (RSF) features excellent biocompatibility and high-strength mechanical properties. However, traditional RSF-based materials can hardly be applied in 3D printing, which has shown great potential in producing artificial implants. In this work, we report a 3D printable RSF hydrogel formed by a weak, chemically crosslinked network. After the 3D printing process, the mechanical properties of the above hydrogel can be remarkably improved by a ripening process. The maximum compressive modulus of this RSF hydrogel is 2.5 MPa, reaching the same order of magnitude as natural elastomers such as cartilage. The mechanical properties of this hydrogel are superior to most RSF-based 3D printed hydrogels. The investigation of gelation mechanism reveals that the chemically crosslinked network can constrain the growth of β-sheet structures of RSF to form a dense and uniform physical network. Such a physically crosslinked network endows the high strength and good resilience of RSF hydrogels. With both good biocompatibility and mechanical properties, this double-network hydrogel has potential in producing 3D printed scaffolds for tissue engineering.
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