In this study, the simultaneous sorption of Cu2+ and p-cresol, which are frequently encountered together in waste waters, into Mg–Al hydrotalcite-like compound (HTlc) modified with dodecylsulfate and ethylenediaminetetraacetate ions (SDS–EDTA-HTlc) was described and compared to a single adsorbate situation. Modification can decrease the specific surface area of the Mg–Al HTlc but promote the sorption for Cu2+ and p-cresol, respectively. Pseudo-second order equations were fitted to the kinetic data, and the rate constants were evaluated. The effect of pH on the simultaneous sorption efficiency was also studied. Freundlich isotherm model was used to analyze the equilibrium data for each adsorbate in both single and binary systems. In binary mixtures, competition for binding sites was identified. The equilibrium Cu2+ uptake decreased with an increased initial p-cresol concentration, whereas the existence of Cu2+ in the solution enhanced the p-cresol removal.