1 Introduction Silkworm silk fibers, an attractive natural biopolymer, possess combined merits of exceptionally strong mechanical properties, scalable renewability, flexible processability, and splendid amphiphilicity.[1] Natural silkworm silk fibers are consisted of thick microfibrils (20–200 nm), which are assembled from bundles of interlocking nanofibers with a diameter of ≈3 nm.[2] Within each silk nanofiber (SNF), the hydrophobic β-crystallites embedded in hydrophilic amorphous matrix...