Organisms use gene and cell engineering to tailor the mineralization process and synthesize structure composites with special functions and favorable properties. This spurs scientists to design functional materials based on learning from nature. Herein, a systematic review of the biomimetic synthesis and hierarchical structure design of calcium carbonate–based minerals is presented. First, biomimetic synthesis strategies, including additive‐induced, template‐oriented, and gel‐mediated routes to direct the construction of the hierarchical structure, are reviewed. The molecular‐recognition technique and directional assembly pathway are then summarized to precisely describe the interactions between inorganic minerals and organic matter, and direct the mineral growth. Next, the underlying mineralization mechanisms governing the evolution of the complex morphology and structure are discussed. Nonclassical pathways that control mineral growth, including the theories of the amorphous phase, oriented attachment, mesocrystal formation, and liquid precursor, are concluded. Finally, herein, the applications of calcium carbonate–based minerals are discussed. Unique hierarchical structure endows minerals with special functions, including optical performance, biomedical applications, and environmental and ecological restoration. Overall, in this report, the biomimetic synthesis of calcium carbonate–based minerals is reviewed, covering the fundamental principles, construction of the hierarchical structure, underlying mechanisms of mineral growth, and functional designs.