Effect of pH on the sorption and desorption of the chlorinated phenols (2-chlorophenol and 2,4-dichlorophenol) in HDTMA-montmorillonite organoclays was investigated using sequential batch experiments. 2,4-dichlorophenol exhibited higher affinity in both sorption and desorption than 2-chlorophenol at pH 4.85 and 9.15. For both chlorophenols, the protonated speciation (at pH 4.85) exhibited a higher affinity in both sorption and desorption than the predominant deprotonated speciation (about 80% and 95% of 2-chlorophenate and 2,4-dichlophenate anions at pH 9.15, respectively). Desorption of chlorinated phenols was strongly dependent on the current pH regardless of their speciation during the previous sorption stage. No appreciable desorption resistance of the chlorinated phenols was observed in organoclays after sequential desorptions. Affinity of both chlorophenols in bisolute competitive sorption and desorption was reduced compared to that in a single-solute system due to the competition between solutes. The ideal adsorbed solution theory coupled with the single-solute Freundlich model successfully predicted the bisolute competitive sorption and desorption equilibria.