Abstract: The adsorption of the monovalent organic cations benzyltrimethylammonium (BTMA) and benzyltriethylammonium (BTEA) to montmorillonite was studied as a function of their concentrations and ionic strength. At low ionic strength the adsorbed amounts of BTMA and BTEA reached values of the cation exchange capacity (CEC) of the clay. An increase in the ionic strength resulted in reduction in the adsorbed amounts of the organic cations, unlike the pattern observed previously with organic monovalent cationic dyes. The reduction in adsorbed amounts of BTMA and BTEA depended on the inorganic cations according to the sequence Cs+ > Na+ > Li+, which follows the sequence of binding coefficients of these inorganic cations added. The type of the anion (that is, Cl− , ClO4−, SO42−) had no effect on the adsorbed amounts. An adsorption model which considers the electrostatic Gouy-Chapman equations, specific binding and closeness of the system could adequately simulate the adsorbed amounts of BTMA and BTEA and yield predictions for the effect of the ionic strength and concentration of electrolytes. The binding coefficient employed was K = 5000 M−1 for the formation of neutral complexes of BTMA and BTEA. This value is larger than those found for the inorganic cations but is several orders of magnitude below those found for the monovalent dyes. The binding coefficients for the formation of charged complexes of BTMA and BTEA were 20 and 5 M−1, respectively. The basal spacing of the clay did not change significantly with the adsorbed amounts of both BTMA and BTEA up to the CEC.