(A) Ashby plot to illustrate the properties of silk fibers in comparison with other materials. Adapted with permission from ref 177. Copyright 2010 American Chemical Society. An opportunity exists to use the material platform of silk, apply the principles that lead to its remarkable properties in carbon materials (graphene, carbon nanotubes, and other materials), and achieve a material performance that features high specific energy to failure at a high specific strength. (B) Synergetic integrations of multiscale modeling, silk polymer synthesis, and microfluidic fiber spinning to study the hierarchical structure of silk polymers and their self-assembly process.