Plasmonic nanocrystals with intrinsic chirality are becoming a hot research focus and offer a wide range of applications in optics, biomedicine, asymmetric catalysis, and enantioselective sensing. Making use of the enantioselective interaction of the chiral biomolecules and plasmonic nanocrystals, the biomolecules-directed synthesis endows chiral plasmonic nanocrystals with tunable optical properties and excellent biocompatibility. Recent advances in the biomolecule-directed geometric control of intrinsically chiral plasmonic nanomaterials have further provided great opportunities for their widespread applications in many emerging technological areas. The review summarizes the recent progress of biomolecule-directed synthesis and potential applications of chiral plasmonic nanocrystals and discusses their development prospects.