When Louis Pasteur introduced the concept of molecular chirality in his groundbreaking work in 1848, he also questioned what might be the forces for the synthesis of the first asymmetric natural products. A variety of strategies have been introduced over the last eighty years for the controlled synthesis and eventual separation of pure enantiomers, which provides a promising answer for the arising of life in the prebiotic stage. Unfortunately, still, no consensus has been reached to uncover the most likely scenario of how the mirror symmetry is initially broken. Inorganic solids such as minerals, metals, and semiconductors have invoked a popular research interest because they can obtain chirality from surface modification or external fields, and thus endow bioorganic molecules with homochirality. Remarkably high activity and selectivity in enantiospecific separation and asymmetric reactions were reported on various solid catalysts such as Au, Pd, and Fe3O4. This can be explained by either electronic structure chirality or crystal structure chirality. The former assumes that the spin-polarized electrons can be viewed as chiral particles longitudinally and could interact with adsorbed molecules according to the chiral-induced spin selectivity (CISS) mechanism. The latter represents the chirality of the crystal surfaces when their Miller indices (h k l) obey h ≠ k ≠ l ≠ k and h × k × l ≠ 0, for example, the (643) surface of cubic Pt. However, little is known about the chemical effects of pure inorganic compounds with bulk chirality crystal structures.