As one of the most common and fascinating phenomena in nature, chiral biominerals exist at all levels from nanoscale to macroscale and in various biological phyla ranging from low-level plants to high-level invertebrate and vertebrate animals with different important functions. Even in the human body, the mineralized pathological calcium carbonate (vaterite) otoconia of the vestibular organ in the inner ear can be chiral through association with vertigo. However, the mechanisms of how these chiral biominerals formed are still not well understood, although more and more evidence has been shown that the biomineralization of chiral biominerals is a crystallization process combined with chiral biomolecular regulations. In this chapter, we first document the crystallization theories including classical and nonclassical models, which have been found in the biomineral formation and biomimetic mineral synthesis. Then, we expound on how these crystallization models are applied in the formation of chiral natural and synthetic biominerals and detail how chiral biomolecules transfer their chirality to biominerals in the crystallization process. This work may provide a comprehensive understanding of the mechanisms of how the complex biomineral suprastructures are formed and advance the development of advanced functional materials.