In this study, novel chitosan-g-itaconic acid/bentonite (CTS-g-IA/BT) and chitosan/bentonite (CTS/BT) nanocomposites were synthesized for adsorption of methylene blue (MB) from aqueous solution. The process was pH-sensitive and maximum sorption was obtained at pH 6 (CTS-g-IA/BT) and 7 (CTS/BT) in 76 h agitation time using 0.03 g of nanocomposites for 50 mL of MB solution. The results showed that in pH less than 6, the adsorption capacity of CTS-g-IA/BT nanocomposite due to the existence of IA monomer is less than that of CTS/BT nanocomposite. The Fourier transform infrared spectroscopy (FTIR) spectrum of CTS-g-IA/BT revealed that both itaconic acid and BT present in the nanocomposite structure, and also the -OH groups of BT, -NH and -OH of CTS participated in nanocomposite formation. According to the FTIR results, a schematic diagram of the nanocomposite synthesis was presented. The kinetic results indicated that the adsorption of MB fitted well with the pseudo-second-order kinetic model. The equilibrium data followed Langmuir isotherm with the maximum adsorption capacity of 500 and 181.818 mg/g for CTS-g-IA/BT and CTS/BT nanocomposites, respectively. The negative values of Gibbs free energy change (ΔG) and the positive values of ΔH confirmed that the adsorption process is spontaneous and endothermic. The positive values of ΔS suggested the randomness of adsorption at interface.