Intermolecular interactions between natural polysaccharides and silk fibroin protein

► Interactions between natural polysaccharides and silk were systematically studied. ► Hydrogen bonding, electrostatic interactions and covalent bonding are focused on. ► The effect of these interactions on structures and properties was investigated. ► Such interactions can change the conformation of silk fibroin protein. ► They can also improve physical and chemical properties of the polymer matrix. Fabricating novel functional and structural materials from natural renewable and degradable materials has attracted much attention. Natural polysaccharides and proteins are the right natural candidates due to their unique structures and properties. The polysaccharide-protein composites or blends were widely investigated, however, there are few systematical studies on the interactions between natural polysaccharides and silk fibroin protein at the molecular level. Among various interactions, hydrogen bonding, electrostatic interactions and covalent bonding play important roles in the structure and properties of the corresponding materials. Therefore, the focus is placed on the three interactions types in this review. A future challenge is to create polysaccharide and protein composites or blends with tailored structure and properties for the wide applications.