Calcite and aragonite are polymorphs with the chemical formula CaCO3. In this study, natural limestone and aragonite, as well as scallop and clam shells composed of calcite and aragonite, were used as the pH-raising neutralizing agents for model solutions containing various heavy metals such as Cd, Cu, Fe, Mn, and Zn to simulate acidic drainage. According to the experimental results, pH-raising effect is higher in the shell materials compared to natural ores for both the calcite and aragonite types. Natural calcite and scallop shells are found to be the most suitable media for Cd removal, while over 95% efficiency for Cu and Fe removal was observed in all four media. Zn removal efficiency is higher in aragonite and clam shells, while Mn removal efficiency is relatively low, to be below 50%, for all four media. Overall, the heavy metal removal efficiency, except for Mn, was over 90%, in the order of Fe > Cu > Cd > Zn > Mn.