Two natural limestone samples, collected from the Campanian-Maastrichtian limestones, Tunisia, were used as adsorbents for the removal of toxic metals in aqueous systems. The results indicated that high removal efficiency could be achieved by the present natural limestones. Among the metal ions studied, Pb2+ was the most preferably removed cation because of its high affinity to calcite surface. In binary system, the presence of Cu2+ effectively depressed the sorption of Cd2+ and Zn2+. Similarly Cu2+ strongly competed with Pb2+ to limestone surface. In ternary system, the removal further decreased, but considerable amount of Pb2+ and Cu2+ still occurred regardless of the limestone sample. The same behavior was observed in quadruple system, where the selectivity sequence was Pb2+ > Cu2+ > Cd2+ > Zn2+. From these results, it was concluded that the studied limestones have the required technical specifications to be used for the removal of toxic metals from wastewaters. © 2012 The Author(s).