New gemini surfactant, glycol bis-N-tetradecyl nicotinate dibromide (designated E-G), and the corresponding monomer, methyl N-tetradecyl nicotinate bromide (E-S), were synthesized and utilized to modify sodium bentonite (Na-Bt). E-G-Bt and E-S-Bt, the surfactant modified bentonites, were then used for methyl orange (MO) removal from the dye solution. E-G was more effective than E-S at expanding the interlayer space of Na-Bt. The adsorption of E-G, E-S and MO obeyed well the pseudo-second-order kinetic model and Langmuir isotherms on Na-Bt or on the modified bentonite. However, the adsorption of E-G was more spontaneous than that of E-S, and E-G replaced more small particles, such as Na+ and water, than E-S did during the adsorption on Na-Bt. The elevated temperature impairs the adsorption of the surfactants, but enhances that of MO. MO absorbed more easily on E-G-Bt than on E-S-Bt. When the dosage of the surfactants used goes beyond a certain amount, the uptake of MO by E-G-Bt/E-S-Bt decreases slowly owing to desorption of the surfactants. E-G and E-S formed a complex with MO on the modified bentonite as UV-vis spectra, and E-G exhibited the stronger interaction with MO. evidenced by