To improve the performance of polyurethane films, small amounts of cellulose nanofibrils (CNF) were physically blended with a waterborne polyurethane (WPU) emulsion, and then CNF/WPU composite films were prepared by cast-coating and drying. The particle size of the emulsions and the chemical structure, micromorphology, thermal stability, mechanical properties, and water resistance of the composite films were characterized using a Malvern laser particle size analyzer, Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), thermogravimetric analysis (TGA), an electronic strength machine, water contact angle analysis (WCA), and water absorption tests, respectively. The results showed that at a low CNF content of 0.3 wt% , the particle size of the WPU emulsion and chemical structure of the film did not change significantly. In addition, the tensile strength of the composite film increased by up to 108% compared to the neat WPU film, and the thermal stability and water resistance were slightly improved. The addition of CNF greatly enhanced the tensile strength while maintaining the other original properties of the WPU film, which may greatly improve the service life and tear resistance of commercial coatings in the future.