a1 Department of Zoology, University of Oxford, UK; email@example.com
a2 Department of Zoology, University of Oxford, UK; firstname.lastname@example.org
a3 Department of Zoology, University of Oxford, UK, and Department of Materials Science and Engineering, University of Sheffield, UK; email@example.com
Comparative silk research has begun to provide us with valuable insights into a class of biopolymers that have evolved an enormous range of material performance based on highly adapted structure-property interactions. As outlined in this article, such insights cover the analysis of biological and bioinspired spinning technologies, the discovery of a novel type of melt spinning at ambient temperatures, and an advanced predictive modeling framework that uses ab initio calculations. Importantly, the huge diversity and extensive range of material properties found in natural silks is providing a fertile field for discoveries that could change the polymer paradigm and our approach to using proteins as structural materials. For example, highly relevant to both sustainability and engineering properties is the role of water in silk processing and function, as this article will explore in some detail.