Helical structures such as double helical DNA and the α-helical proteins found in biological systems are among the most beautiful natural structures. Chiral nanoarchitectonics, which is used here to describe the hierarchical formation and fabrication of chiral nanoarchitectures that can be observed by atomic force microscopy (AFM), scanning tunneling microscopy (STM), scanning electron microscopy (SEM), or transmission electron microscopy (TEM), is one of the most effective ways to mimic those natural chiral nanostructures. This article focuses on the formation, structure, and function of the most common chiral nanoarchitectures: nanoscale chiral twists and helices. The types of molecules that can be designed and how they can form hierarchical chiral nanoarchitectures are explored. In addition, new and unique functions such as amplified chiral sensing, chiral separation, biological effects, and circularly polarized luminescence associated with the chiral nanoarchitectures are discussed.