The sorption of lead (II) and cadmium (II) on seven shales belonging to the Proterozoic Vindhyan basin, central India, and a black cotton soil, Mumbai, India, was studied and compared with sorbent geochemistry. The sorption equilibrium studies were conducted under completely mixed conditions in batch reactors (pH=5.0 and ionic strength= 0.01 M) at room temperature. The Freundlich model provided better fits to the experimental data compared to Langmuir model. High cadmium and lead sorption was observed for the calcareous shales with greater than 5% CaCO3. The Freundlich isotherm parameter relating to sorption capacity, i.e., KF, yielded a strong correlation with the calcium carbonate and calcium oxide content across the various geosorbents studied. The observed sorption pattern may be attributed to complex formation of CaCO3 with Pb2+ and Cd2+ leading to surface precipitation. Moreover, the Ca2+ present in the sorbents may also involve in ion exchange reaction with lead and cadmium.