It is of great academic value to study the influence of carbonate doping on the growth behavior of synthetic diamond crystals. In this paper, CaCO3 was doped into the carbon source in the diamond synthesis cavity at different ratios using the temperature gradient method at high pressure and high temperature (HPHT). The purpose of the study is to investigate the effect of CaCO3 doping on the growth behavior of diamond along the (100) or (111) crystal plane, respectively. The crystal morphology of doped synthetic diamonds was studied by optical microscopy. The results show that with the increase of the CaCO3 content, the crystal shape of diamond growing along the (100) plane change from tower to plate accompanied by crack crystal or crystals stock. The color of the crystal becomes lighter and then darker, and the inclusions appear in diamond. Besides, the crystal shape of diamond growing along (111) surface gradually changes from plate to tower accompanied by crack and twin crystals phenomena. With the increase of the CaCO3 content, the color of diamond crystals gradually becomes darker, and more inclusions appear in diamond. The Raman spectroscopy results show that with the increase of CaCO3 content, the Raman peak position shifts of doped diamond growing along (100) or (111) plane increase, and the full width at half maximum (FWHM) becomes larger. This indicates that the doping of CaCO3 increases crystal lattice distortion and internal stress of diamond. In this paper, the causes for the effect of CaCO3 doping on the crystal shape, color, internal quality and other behaviors of the diamond growing along the two different faces were analyzed, which lays the foundation for the subsequent study of this topic.