Graphene oxide (GO)-based composite materials have become widely popular in many applications due to the attractive properties of GO, such as high strength and high electrical conductivity at the nanoscale. Most current GO composites use organic polymer as the matrix material and thus, their synthesis suffers from the use of organic solvents or surfactants, which raise environmental and energy-consumption concerns. Inspired by mussel foot proteins (Mfp) secreted by the saltwater mussel, Mytilus galloprovincialis and by recent advances in microbial protein production, we developed an aqueous-based green synthesis strategy for preparing GO/Mfp film composites. These GO/Mfp films display high tensile strength (134-158 MPa), stretchability (~ 26% elongation), and high toughness (20-24 MJ/m3), beyond the capabilities of many existing GO composites. Renewable production of Mfp proteins and the facile fabrication process described provides a new avenue for composite material synthesis, while the unique combination of mechanical properties of GO/Mfp films will be attractive for a range of applications.