Biopolymers show a broad prospect as an effective alternative to petroleum-based materials. However, assembling biopolymers into the composites with integrated high strength and toughness still remains a great challenge. Herein, we developed a novel and versatile mussel-inspired modification design for tough and high-performance graphene oxide (GO)/soy protein isolate (SPI) nanocomposite films, where the GO nanosheets were modified with poly(dopamine) (PDA) to improve the dispersion of GO nanosheets in SPI matrix and enhance their interfacial adhesion. As expected, at 0.6 wt% of PDAmodified GO (PDG) loading, the tensile strength and toughness of the SPI/PDG films reached 8.87 MPa and 22.82 MJ m(-3), respectively, which simultaneously showed 86.34% and 263.95% higher than those of pristine film. The great enhancement of mechanical behaviors was due to the increased fracture line energy and the lack of significant coalescence of microcracks, as well as the strong interfacial adhesion force between peptide chains and PDG nanosheets. The resultant nanocomposite films also exhibited favorable vapor barrier behavior and water-resistance. The proposed method in this paper opens a new avenue for assembling two-dimensional nanosheets into the biopolymer-based composites with integrated high strength and great toughness for a series of innovative future applications. (C) 2018 Published by Elsevier B.V.