Two novel modified montmorillonite (Mnt) components were prepared using Mnt nanoparticles and two surfactants: docosyl-trimethylammonium chloride (BTAC) and sodium dodecyl sulfate (SDS). These modified Mnts were used to remove a carcinogenic and harmful dye, crystal violet (CV), from solution. Optimization and modelling studies of the adsorption of these two modified Mnts were performed using response surface methodology. Four influential variables (concentration of adsorbent, temperature, pH and CV concentration) were studied to obtain the optimum conditions for CV removal. The optimal values of these variables for the two modified Mnts yielded 100% dye-removal efficiency. The optimum conditions for CV adsorption on Mnt-BTAC and Mnt-BTAC-SDS, respectively, are temperatures of 25.00 and 33.29°C, pH values of 9 and 10.1, CV concentrations of 50.00 and 10.44 mg L–1 and adsorbent concentrations of 1.00 and 0.98 g L–1. In equilibrium studies of the two modified Mnts, the Temkin isotherm was selected as an appropriate model, and in kinetic studies of these Mnts, the fractal-like integrated kinetics Langmuir model was found to be the best model. The Mnt-BTAC-SDS component is an affordable adsorbent with high adsorption capacity for CV.