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Animal silks, consisting of pure protein components, offer an extraordinary combination of strength, elongation, and toughness, exceeding most engineered materials. The secret to this success is their unique nanoarchitectures formed through the hierarchical self‐assembly of silk proteins. This natural process contrasts the production of artificial silk materials, which usually are directly constructed as bulk structures from silk fibroin (SF) molecules. A variety of fabrication strategies to control nanostructures of silks or to create functional materials from silk nanoscale building blocks have been developed in the recent years. 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. Herein, the critical roles of silk nanoarchitectures in property and function of natural silk fibers are reviewed and the strategies of utilization of these silk nanobuilding blocks are outlined. Further, the state‐of‐the‐art techniques to create silk nanoarchitectures and to generate silk‐based nanocomponents are summarized. An effective approach to constructing sophisticated silk functional nanocomposites with promising applications in regenerative medicine, drug delivery, and optical and electronic device designs is provided. Further, such insights suggest templates to consider for other material systems.

Patterning of photonic crystals to generate rationally designed color‐responsive materials has drawn considerable interest because of promising applications in optical storage, encryption, display, and sensing. Here, an inkjet‐printing based strategy is presented for noncontact, rapid, and direct approaches to generate arbitrarily patterned photonic crystals. The strategy is based on the use of water‐soluble biopolymer‐based opal structures that can be reformed with high resolution through precise deposition of fluids on the photonic crystal lattice. The resulting digitally designed photonic lattice formats simultaneously exploit structural color and material transience opening avenues for information encoding and combining functions of optics, biomaterials, and environmental interfaces in a single device.

Hierarchical molecular assembly is a fundamental strategy for manufacturing protein structures in nature. However, to translate this natural strategy into advanced digital manufacturing like three‐dimensional (3D) printing remains a technical challenge. This work presents a 3D printing technique with silk fibroin to address this challenge, by rationally designing an aqueous salt bath capable of directing the hierarchical assembly of the protein molecules. This technique, conducted under aqueous and ambient conditions, results in 3D proteinaceous architectures characterized by intrinsic biocompatibility/biodegradability and robust mechanical features. The versatility of this method is shown in a diversity of 3D shapes and a range of functional components integrated into the 3D prints. The manufacturing capability is exemplified by the single‐step construction of perfusable microfluidic chips which eliminates the use of supporting or sacrificial materials. The 3D shaping capability of the protein material can benefit a multitude of biomedical devices, from drug delivery to surgical implants to tissue scaffolds. This work also provides insights into the recapitulation of solvent‐directed hierarchical molecular assembly for artificial manufacturing.