In this study, novel active films based on pullulan and carboxylated cellulose nanocrystal (C-CNC) incorporated with tea polyphenol (TP) was prepared by solution casting method. The effect of TP addition on the microstructural, mechanical, barrier, optical, functional properties of the resultant pullulan/C-CNC/TP (PC-TP) bionanocomposite films was systematically evaluated. Scanning electron microscopy showed that an appropriate TP adding was well distributed within the PC-TP bionanocomposite matrix. Fourier-transform infrared further revealed that new hydrogen bond was formed among the pullulan, C-CNC, TP. Addition of TP at an appropriate level (3%, w/w, on a dry basis of the weight of pullulan and C-CNC) led to stronger intermolecular interactions and more compact microstructure, and thus enhanced the water barrier properties, thermal stability and tensile strength of the resultant bionanocomposite films. Nevertheless, overloading of TP in the bionanocomposite films might produce some aggregations and thus have negative effects on their performance. In addition, the incorporation of TP significantly improved the UV-barrier properties, antioxidant activity and antimicrobial activity of PC-TP bionanocomposite films, while induced a decrease in the transmittance. These results revealed that PC-TP bionanocomposite films with TP at appropriate levels had potential to be used as active food packaging.