In this paper, composite fillers including graphene oxide and carbon black had been applied to modify pure waterborne polyurethane (WPU) and a new nanocomposite was prepared by in situ polymerization, whose structure was characterized by Fourier transform infrared spectroscopy that demonstrated interfacial interactions existing between the filler particles and the hard segments of WPU chains. Meanwhile, thermal properties of prepared nanocomposites were enhanced after adding composite fillers as shown in the results of thermogravimetric analysis and differential scanning calorimetry curves, which could be explained by several factors including strong interface interaction between organic phase and inorganic phase verified by infrared spectra and scanning electron microscopy as well as transmission electron microscopy, good dispersion and barrier effect of the composite fillers, reinforced crosslinking density of the system. Additionally, the contact angle and anticorrosion performance of the nanocomposite films were heightened after adding fillers. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020, 137, 48716.