The main objective of this work was to evaluate the potential of Montmorillonite nanoclay (Mt), readily and inexpensively available, for the simultaneous adsorption (and removal) of two classes of pollutants: metal ions and dyes. The attention was focused on two “model” pollutants: Ce(III) and crystal violet (CV). The choice is due to the fact that they are widespread in wastewaters of various origins. These characteristics, together with their effect on human health, make them ideal for studies on water remediation. Moreover, when separated from wastewater, they can be recycled individually in industrial production with no or simple treatment. Clay/pollutant hybrids were prepared under different pH conditions and characterized through the construction of the adsorption isotherms and powder X-ray diffraction. The adsorption behavior of the two contaminants was revealed to be significantly different: the Langmuir model reproduces the adsorption isotherm of Ce(III) better, thus indicating that the clay offers a unique adsorption site to the metal ions, while the Freundlich model proved to be the most reliable for the uptake of CV which implies heterogeneity of adsorption sites. Moreover, metal ions do not adsorb at all under acidic conditions, whereas the dye is able to adsorb under all the investigated conditions. The possibility to modulate the adsorption features by simply changing the pH conditions was successfully employed to develop an efficient protocol for the removal and separation of the different components from aqueous solutions mimicking wastewaters.