Adsorption of cationic methylene blue and anionic orange II onto unmodified and surfactant-modified zeolites was studied using a batch equilibration method. The effects of equilibrium time, solution pH, and sorption temperature were examined. The results suggested that 2% sodium dodecyl benzenesulfonate (SDBS)- and 3% sodium dodecyl sulfate (SDS)-modified zeolites had higher adsorption capacities for methylene blue than the unmodified zeolite, while 2% cetylpyridinium bromide hexadecyl (CPB)- and 2% hexadecylammonium bromide (HDTMA)-modified zeolites were the best adsorbents for orange II. The adsorption conditions were optimized, and the mechanisms of adsorption are briefly discussed.