Using muscovite as the carrier, TiCl4 as the source of titanium, urea as the precipitating agent, nano-TiO2/mica photocatalyst (TiO2/M) was prepared by the method of hydrolysis–precipitation. The as - prepared photocatalyst was characterized by XRD, SEM, EDS and UV methods. The methyl orange was used as contamination simulation to test the photocatalytic activity of the materials. The influence of the calcination temperature, radiation time and photocatalyst adding amount on photocatalytic activity of methyl orange were also discussed. The SEM and XRD results showed that nano-TiO2 particles had been evenly coated on the muscovite surface to be a dense layer. The results showed that: the phases of as – prepared materials were mixed crystalline of anatase and rutile after calcinating from 400°C to 700°C; After calcinating at 400°C for 2h, and adding concentration was 2g/L, the material had the best photocatalytic activity, the degradation rate of methyl orange reached 98% after radiation under 300W mercury lamp for 60min.