To better predict the fate and mobility of surfactants in the environment, sorption and desorption of a nonionic polyoxyethylene lauryl ether surfactant (Brij 35) by two smectites (Wyoming montmorillonite and Panther Creek smectite) and two interstratified mica-vermiculites (IMVs) were investigated by batch techniques, X-ray diffraction, and infrared spectroscopy. Maximum surfactant sorption by smectites ranged from 196 to 256 g kg−1, whereas the maximum sorption by the IMVs was indeterminate over the range of concentrations employed. Sorption by smectites was best described by the Langmuir model, but sorption by the IMVs showed an S-shaped isotherm, suggesting that cooperative sorption occurred. The surfactant was more readily desorbed from the IMVs than from the smectites in an initial wash with water. After two water washes, 65–75% of the initially sorbed surfactant was retained by the smectite, and 44–51% of the surfactant sorbed to the IMVs remained with the solid phase. In this study, basal spacing of the smectites increased to ~17.5 Å near the sorption maximum, suggesting intercalation of surfactant molecules in the interlamellar regions of the clay. X-ray data also suggested that the surfactant molecules were oriented horizontally in the interlayer spaces. Greater surfactant sorption by the Ca-smectites gradually diminished the intensity of the 1630 cm−1 infrared band dues to hydration water, indicating that some water had been displaced by the surfactant. The surfactant was also sorbed by the IMV clays, but only on external surfaces and probably via interactions of micelles with the solid phase.