The paper prepares the intercalated CTMA-bentonite by Na-bentonite cation exchanged with cetyltrimethylammonium and characterizes the product by XRD and IR techniques. The d001 spacing value of CTMA-bentonite is 7.54 larger than that of Na-bentonite at 100% of the cation exchange capacity. The IR spectrum shows that the intensities of OH stretching and bending vibrations of CTMA-bentonite decrease greatly compared with the untreated Na-bentonite. Batch experiments are carried out at 303 K, 323 K and 343 K to obtain the sorption isotherms of methyl orange on CTMA-bentonite. The results show that the sorption isothermal data can be well described by Langmuir and Freundlich model accurately. The dynamical data fit well with pseudo-second-order kinetic model. Thermodynamic parameters such as changes in the free energy (ΔG0), the enthalpy (ΔH0) and the entropy (ΔS0) are also evaluated. The overall adsorption process of methyl orange on CTMA-bentonite is spontaneous, exothermic physisorption. The CTMA-bentonite can be employed as low-cost alternatives to activated carbon in wastewater treatment for the removal of corlor which comes from textile dyes.