Using employed FeCl3 as oxidant and dopant, polypyrrole(PPy)/attapulgite (ATP) nanocomposites were prepared by in situ polymerization to remove high poisonous Cr6+ions from aqueous solutions. The results indicate that the adsorbent possesses high adsorption speed and can reach the adsorption equilibrium within 10min. Other influencing factors such as adsorbent dose, initial concentration of Cr6+ and pH value were investigated. Isotherm data fits well to the Langmuir isotherm model. The maximum adsorption capacity for Cr6+ is 48.45mg/g. The thermodynamic parameters, ΔH, ΔG, ΔS were evaluated. Thermodynamic parameters are all negative which imply that the adsorption process is spontaneous and exothermic. The adsorption process follows pseudo-second-order equation, which indicates the adsorption process is controlled by chemical adsorption mechanism. The composites were characterized by Fourier transform infrared spectra(FT-IR) and scanning electron microscopy(SEM). The results suggest that surfce of ATP was covered with PPy to form nanocomposites.