Spherical CoCO3 powder with a small particle size and high density was successfully prepared using a continuous carbonate liquid precipitation method with a raw material of cobalt chloride solution, a precipitant of NH4HCO3, and without a template. The effects of the concentration of ammonium carbonate, process pH, and feeding rate on the tap density and apparent density of cobalt carbonate were investigated. It was found that the apparent and tap density values of 4.4 µm of cobalt carbonate were 1.27 g/cm3 and 1.86 g/cm3, respectively, when the initial concentration of NH4HCO3 solution was 60 g/L, the pH was 7.15–7.20, and the feeding rate of cobalt chloride was 2 L/h. The anisotropic growth process of the crystal lattice plane of CoCO3 under the aforementioned optimal conditions were studied. The results demonstrated that the crystal grew fastest along the (110) facet orientation, which was the dominant growth surface, determining the final morphology of the primary particles. The scanning electron microscopy (SEM) and high-resolution transmission electron microscopy (HR-TEM) results demonstrated that the primary particle morphology of the cobalt carbonate was a nanosheet. The unit cell of cobalt carbonate, of a hexagonal structure in the horizontal direction, grew horizontally along the (110) facet orientation, while 20–35 unit cells of the carbon carbonate were stacked along the c-axis in the thickness direction. Finally, the sheet-shaped particles were agglomerated into dense spherical secondary particles, as presented through the crystal re-crystallization model.