A facile, inexpensive, and green approach for the production of stable graphene dispersion was proposed in this study. We fabricated soy protein isolate (SPI)-based nanocomposite films with the combination of 2D negative charged graphene and 1D positive charged polyethyleneimine (PEI)-modified cellulose nanocrystals (CNC) via a layer-by-layer assembly method. The morphologies and surface charges of graphene sheets and CNC segments were characterized by atomic force microscopy and Zeta potential measurements. The hydrogen bonds and multiple interface interactions between the filler and SPI matrix were analyzed by Attenuated Total Reflectance–Fourier Transform Infrared spectra and X-ray diffraction patterns. Scanning electron microscopy demonstrated the cross-linked and laminated structures in the fracture surface of the films. In comparison with the unmodified SPI film, the tensile strength and surface contact angles of the SPI/graphene/PEI-CNC film were significantly improved, by 99.73% and 37.13% respectively. The UV–visible light barrier ability, water resistance, and thermal stability were also obviously enhanced. With these improved functional properties, this novel bio-nanocomposite film showed considerable potential for application for food packaging materials.

This study applied a facile and green approach to synthesize a stable graphene aqueous dispersion, and the graphene aqueous dispersion was employed to modify the renewable, compatible and biodegradable soy-protein-isolated (SPI) films to enhance their thermal stability, mechanical properties and water resistance. Atomic force microscopy (AFM) images confirmed the monolayer structure of graphene. The hydrogen bonds and π–π interactions between graphene and the SPI molecules were showed with the attenuated total reflectance Fourier transform infrared (ATR FT-IR) spectroscopy, and X-ray diffraction (XRD). As expected, compared to the pure SPI film, the tensile strength (TS) of the film with 74% graphene increased by 27.22% and the total soluble matter (TSM) of the film with 93% graphene decreased by 11.30%.