A simple and convenient method for preparing visible light response photocatalyst polypyrrole/TiO2 (PPy/TiO2) nanocomposite was developed. The products were characterized by x-ray diffraction, transmission electron microscopy, atomic force microscopy, ultraviolet-visible, and Fourier transform infrared techniques. The results indicated that the nanohybrid was composed of anatase TiO2 and PPy and exhibited an enhanced visible light-capturing ability. Average diameters of TiO2 and PPy/TiO2 were 18 and 35 nm, respectively. The photocatalytic activity of the nanocomposite was evaluated by the degradation of methyl orange under visible light irradiation. In the presence of PPy/TiO2 nanocomposite, the degradation efficiency of methyl orange of 95.54% could be obtained under visible light irradiation within 120 min. The apparent rate constant was 2.19 × 10−2, which was better than that Degussa P25 nano-TiO2. The sensitization mechanism of PPy/TiO2 photocatalyst was discussed briefly.