The behavior of different acid zeolites in the hydrolysis at room temperature of methyl tert-butyl ether (MTBE) was studied with reference to the possibility of its conversion to more biodegradable products in underground water contaminated by MTBE. The effect of the structure of the zeolite and SiO2/Al2O3 ratio was analyzed. The results indicate that acid H-MFI and H-BEA zeolites are effective in both adsorption and hydrolysis of MTBE and may be applied for both in situ underground water remediation and as protection barrier for wells or leaking tanks. However, other zeolites (mordenite and faujasite) result completely inactive. Furthermore, contrary to what was expected, the increase of the Si/Al ratio promotes the reactivity which is determined by the resistance to diffusion of MTBE in the pores of zeolites and the resistance of back-diffusion of the reaction products.