Silk fibroin has applications in different medical fields such as tissue engineering, regenerative medicine, drug delivery and medical devices. Advances in silk chemistry and biomaterial designs have yielded exciting tools for generating new silk-based materials and technologies. Selective chemistries can enhance or tune the features of silk, such as mechanics, biodegradability, processability and biological interactions, to address challenges in medically relevant materials (hydrogels, films, sponges and fibres). This Review details the design and utility of silk biomaterials for different applications, with particular focus on chemistry. This Review consists of three segments: silk protein fundamentals, silk chemistries and functionalization mechanisms. This is followed by a description of different crosslinking chemistries facilitating network formation, including the formation of composite biomaterials. Utility in the fields of tissue engineering, drug delivery, 3D printing, cell coatings, microfluidics and biosensors are highlighted. Looking to the future, we discuss silk biomaterial design strategies to continue to improve medical outcomes.
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