Several polyacrylonitrile (PAN)/tea polyphenol (TP) blends were prepared with various mixing weight ratios (percentage). With a commercial acrylonitrile–butadiene–styrene (ABS) as reference, the results show that the PAN/TP blends with 12.5 wt % TP had a better antiwear ability and similar hardness to those of ABS. All of the prepared PAN/TP blends showed a lower impact strength than the referenced ABS. However, some values were indeed higher than those reported for engineering materials in the literature, for example, polystyrenes and some ABS blends. Differential scanning calorimetry, differential thermogravimetry, and dynamic mechanical analysis indicated that the PAN/TP blends had enhanced the thermal stability compared to the pure PAN. Fourier transform infrared spectral analysis suggested that the H bonds increased in the PAN/TP blends. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40411.