Surfactant-modified clinoptilolite-rich tuff was used for the removal of methyl tert-butyl ether (MTBE) from aqueous solutions. Clinoptilolite zeolite from Miyaneh region of Iran was treated with sodium chloride and then modified with hexadecyltrimethylammonium chloride (HDTMA-Cl) and n-Cetylpyridinium bromide (CPB) to be used in different experimental conditions. The ability of raw or Non-Modified Zeolite (NMZ) and Surfactant-Modified Zeolites (SMZ) to remove MTBE from aqueous solutions was investigated as a function of contact time, pH and concentrations of adsorbent and adsorbate, by using a batch technique in aqueous system. The removal of MTBE from aqueous solutions by modified zeolites seemed to be more effective than non-modified samples. Also, HDTMA-modified zeolite had more effective performance than CPB-modified zeolite. The adsorption efficiency of MTBE onto SMZ _S was found to increase by contact time and adsorbent concentrations, and by decreasing of pH and adsorbate concentrations. Empirical adsorption models of Langmuir and Freundlich were applied for the experimental data. Results showed that Langmuir isotherm was more suitable for this process. The experimental data fitted very well with the pseudo-second-order kinetic model. It was overally found that Surfactant-Modified Zeolites is an effective adsorbent for removal of methyl tert-butyl ether from contaminated solutions.