CaCO3 has six polymorphs such as vaterite, aragonite, calcite, amorphous, crystalline monohydrate, and hexahydrate CaCO3. CaCO3 is a typical biomineral that is abundant in both organisms and nature and has important industrial applications. Cellulose could be used as feedstocks for producing biofuels, bio-based chemicals, and high value-added bio-based materials. In the past, more attentions have been paid to the synthesis and applications of CaCO3 and cellulose/CaCO3 nanocomposites due to its relating properties such as mechanical strength, biocompatibility, and biodegradation, and bioactivity, and potential applications including biomedical, antibacterial, and water pretreatment fields as functional materials. A variety of synthesis methods such as the hydrothermal/solvothermal method, biomimetic mineralization method, microwave-assisted method, (co-) precipitation method, and sonochemistry method, were employed to the preparation of CaCO3 and cellulose/CaCO3 nanocomposites. In this chapter, the recent development of CaCO3 and cellulose/CaCO3 nanocomposites has been reviewed. The synthesis, characterization, and biomedical applications of CaCO3 and cellulose/CaCO3 nanocomposites are summarized. The future developments of CaCO3 and cellulose/CaCO3 nanocomposites are also suggested.