A hydroxy-sodalite/cancrinite zeolite composite was synthesized from low-grade calcite-bearing kaolin by hydrothermal alkali-activation method at 160 • C for 6 h. The effect of calcite addition on the formation of the hydroxy-sodalite/cancrinite composite was investigated using artificial mixtures. The chemical composition and crystal morphology of the synthesized zeolite composite were characterized by X-ray powder diffraction, infrared spectroscopy, scanning electron microscopy, and N 2 adsorption/desorption analyses. The average specific surface area is around 17-20 m 2 ·g −1 , whereas the average pore size lies in the mesoporous range (19-21 nm). The synthesized zeolite composite was used as an adsorbent for the removal of heavy metals in aqueous solutions. Batch experiments were employed to study the influence of adsorbent dosage on heavy metal removal efficiency. Results demonstrate the effective removal of significant quantities of Cu, Pb, Ni, and Zn from aqueous media. A comparative study of synthesized hydroxy-sodalite and hydroxy-sodalite/cancrinite composites revealed the latter was 16-24% more efficient at removing heavy metals from water. The order of metal uptake efficiency for these zeolites was determined to be Pb > Cu > Zn > Ni. These results indicate that zeolite composites synthesized from natural calcite-bearing kaolin materials could represent effective and low-cost adsorbents for heavy metal removal using water treatment devices in regions of water shortage.