Structural biopolymers are materials engineered by Nature as building blocks of living matter. These materials have unique and compelling properties that allow for their assembly and degradation with minimal energy requirements as well as their performance at the biotic/abiotic interface. By combining basic material principles with advanced fabrication techniques, it is possible to define new strategies to drive the assembly of structural biopolymers in advanced materials with unconventional forms and functions such as edible coating for perishable food, inkjet prints of silk fibroin that change in color in the presence of bacteria, three dimensional monoliths that can be heated by exposure to infrared light and flexible keratin-made photonic crystals.