“…With the abuse of nonrenewable fossil reserves and the rising environmental concerns, it is highly desirable to convert renewable bioresources into sustainable energy, chemicals, and materials. − Natural polymers (e.g., cellulose, lignin, chitin, chitosan, wool keratin, and silk fibroin), featuring with renewability, abundance, biocompatibility and biodegradability, can be developed as ideal raw sources for preparing eco-friendly bioproducts. − Among them, silk fibroin (SF), a sustainable natural protein material is widely used in the textile and biomedical industries due to its unique properties, such as nontoxicity, low immunogenicity, excellent biocompatibility, and sufficient mechanical properties. − However, the commercial silk textile industry currently requires sorted high-quality cocoons, and thus, tons of silk offcuts and textile waste are generated yearly from spinning mills, processing industries, and cultivated plants, as well as old silk-fabric textiles. − Therefore, the facile use of these SF-based wastes in value-added materials is highly favorable from the perspective of the sustainable development of silk-based industry and society …”