A series of biopolymer chitosan/montmorillonite (CTS/MMT) nanocomposites were prepared by controlling the molar ratio of chitosan (CTS) and montmorillonite (MMT). The nanocomposites were characterized by FTIR and XRD. The effects of different molar ratios of CTS and MMT, initial pH value of the dye solution and temperature on adsorption capacities of samples for Congo Red (CR) dye have been investigated. The adsorption capacities of CTS, MMT and CTS/MMT nanocomposite with CTS to MMT molar ratio of 5:1 for CR were compared. The results indicated that the adsorption capacity of CTS/MMT nanocomposite was higher than the mean values of those of CTS and MMT. The adsorption kinetics and isotherms were also studied. It was shown that all the sorption processes were better fitted by pseudo-second-order equation and the Langmuir equation.