The potentiometric titration and CEC data presented in part I are modeled in this paper, part II. Two models are compared: the two pK, three complexation sites plus exchange sites nonelectrostatic model developed by Baeyens and Bradbury and a model based on the MUSIC approach developed by Hiemstra and Van Riemsdijk. Both morphological and structural information is used to develop this new model. Morphological information is taken from the literature, while structural information is taken from the literature and constrained by supporting FTIR experiments. The Baeyens and Bradbury model is found to reproduce the general tendency of the titration curve, whereas the model based on the Hiemstra and Van Riemsdijk MUSIC approach provides a better fit to the experimental data. The former uses only 3 edge reaction sites, whereas the latter uses at least 27 edge reaction sites. Five main reactive sites are sufficient to fit the MUSIC model curve, but the model allows us to derive the properties of 22 other reactive sites. Logically, the greater the number of sites, the better the fit. Nevertheless, fewer adjustable parameters are necessary for the Hiemstra and Van Riemsdijk MUSIC model than for the Baeyens and Bradbury model, thanks to structural and morphological constraints. The precision of the potentiometric titration curve is insufficient to verify that the properties of the 27 sites given by the MUSIC model are effective. Thus, we coupled some properties of clay minerals, such as dissolution, to the modeled acid–base properties of these sites to assess our model. We then questioned the ability of simplified models such as the Baeyens and Bradbury model to predict the interactions between clay minerals and solutions in natural environments. In addition, we derived the cation exchange selectivity coefficients for CaCl+ ionic pairs and H+ from our CEC data and gave an estimate for the CaOH+ selectivity coefficient.