The dual-mode sorption model (DSM) was applied to the single-solute sorption of 2-chlorophenol, 3-cyanophenol, and 4-nitrophenol from water onto organoclays. The three parameters contained in the DSM were determined for each solute by fitting to the single-solute isotherm data and subsequently utilized in competitive multisolute sorptions. A systematic method to determine the parameters for each solute was also suggested. The ideal adsorbed solution theory (IAST) coupled with the single-solute DSM and the competitive dual-mode sorption model (CDSM) extended to describe multisolute sorption were used to predict multisolute sorption onto organoclays and compared with the data to determine the predictive capabilities. The DSM was found to describe well single-solute sorption from water onto organoclays. The predictions from the CDSM and the IAST based on the DSM, though rather poor for some solutes, were generally in agreement with the multisolute sorption data. However, we could not tell at this stage which of the two competitive models is better.