This article focuses on the synthetic approach to the preparation of calcium carbonate–organic hybrid materials, which are obtained by self‐organization processes under mild conditions. In these processes, organic molecules such as functionalized polymers and aligned amphiphilic molecules on the surface play key roles in the crystallization of calcium carbonate, which results in the formation of hybrid materials. As well as being environmentally benign, the hybrid materials have controlled morphology and unique properties. Materials scientists have obtained the ideas for the design of such hybrid materials from biominerals such as shells, teeth, and bones.