The biological relevance of chirality has aroused significant interest for the modulation of pathological and biomedical activity. With a commensurate size scale to the biological environment, chiral inorganic nanomaterials could exhibit enzyme-like properties that dictate the selectivity and directionality of bioactivity. This chirality-dependent functionality originates from handedness-dependent interactions at chiral organic-inorganic interfaces or chiral light-matter interactions, enabling high-precision molecular analysis and high-efficiency biomedical therapy. This perspective provides an overview of biomolecule-driven chiral inorganic nanomaterial synthesis, enantioselective interactions at organic-inorganic interfaces, and biomedical applications for chirality-dependent molecular sensing and therapeutics. A comparison of representative chiral inorganic nanostructures suggests that nanoscale control of chiral features is critical for enhancing the ultimate chirality in inorganic nanomaterials. Therefore, quantitatively understanding chiral organic-inorganic interfaces and more systematically modulating their relationship, such as systematically incorporating sequence-programmable biomolecules (such as DNA or proteins), have been suggested as a potential direction for research into biomedically functional chiral inorganic nanomaterials.