Design, Fabrication, and Function of Silk‐Based Nanomaterials

Animal silks are built from pure protein components and their mechanical performance, such as strength and toughness, often exceed most engineered materials. The secret to this success is their unique nanoarchitectures that are formed through the hierarchical self-assembly of silk proteins. This natural material fabrication process in sharp contrast to the production of artificial silk materials, which usually are directly constructed as bulk structures from silk fibroin (SF) molecular. In recent years, with the aim of understanding and building better silk materials, a variety of fabrication strategies have been designed to control nanostructures of silks or to create functional materials from silk nanoscale building blocks. These emerging fabrication strategies offer an opportunity to tailor the structure of SF at the nanoscale and provide a promising route to produce structurally and functionally optimized silk nanomaterials. Here, we review the critical roles of silk nanoarchitectures on property and function of natural silk fibers, outline the strategies of utilization of these silk nanobuilding blocks, and we provide a critical summary of state of the art in the field to create silk nanoarchitectures and to generate silk-based nanocomponents. Further, such insights suggest templates to consider for other materials systems.