The calcium carbonate composite particles with nanostructured surface were prepared by heterogeneous nucleation. The calcium carbonate composite particles consisted of a core of groundcalcium carbonate particle and a shell of nanometer calcium carbonate particles. The thickness of theshell of composite calcium carbonate was observed by TEM. The bond intensity between the core and the shell was measured by means of ultrasonic comminution and stirred ball milling. It was found that the composite calcium carbonate had a compact structure. The linkage between the core and shell was so strong that it must be chemical bond instead of physical adsorption.