Removal of heavy metals from water and wastewaters has recently gained a great deal of attention due to their serious environmental problems. In this study, novel synthesized calcium carbonate nanoparticles, prepared in a colloidal gas aphron (CGA) system, were used as adsorbents for the removal of Cu-2 ions from aqueous solutions under different conditions. A developed pseudo-second-order (PSO) model well described the adsorption kinetics of the process. Langmuir and Freundlich adsorption isotherms have been examined and the maximum adsorption capacity from the Langmuir isotherm equation was found to be 666.67 mg Cu/g adsorbent. The effects of temperature, Cu2+ initial concentration, and CaCO3 dosage on the removal capacity were also investigated using the three-level Box-Behnken experimental design method. The response surface modeling results demonstrated that under certain experimental conditions (i.e., T = 26 degrees C, [Cu2+] = 200 mg/L, and [CaCO3] = 0.5 g/L), maximum removal capacity value (393.52 mg/g) was achieved.