Many studies have been conducted to study the various polymorphs and morphologies of calcium carbonate crystals in nature and living organisms. In this experimental work, a novel method has been employed to crystallize calcium carbonate by using colloidal gas aphron dispersion. The polymorph and morphology of prepared particles were investigated using scanning electron microscopy (SEM), X-ray diffraction (XRD), and Fourier transform infrared spectrometry techniques. SEM and XRD analyses demonstrated that the morphology of synthesized CaCO3 can be changed from spherical (vaterite phase) to novel rod and plate-like shapes (mixture of vaterite and calcite phases) with changes in the surfactant concentration. The quantitative examination results of different calcium carbonate polymorph orientations showed that the precursor concentrations had no significant effect on the orientation of calcite phase, but rather they affected the orientation development of vaterite phase at a higher surfactant concentration.