Vibrational circular dichroism (VCD) being a relatively new spectroscopic technique is quite promising for studying of biological molecules and their complexes. It combines conformational sensitivity of electronic circular dichroism (CD, or ECD) with extensive local mode information provided by the vibrational spectroscopy. Another advantage of VCD over ECD is its applicability to complexes of biological macromolecules, which would cause considerable light scattering in the UV region. This makes VCD a particularly useful tool for the investigation and characterization of various molecular structures. Here, we overview the theoretical background, discuss some practical aspects of VCD application to biological molecules, and list major spectral features encountered in the most common types of DNA and protein secondary structures. We also describe VCD applications to structural and conformational analysis of biological macromolecules and their complexes, including those with metal ions and drugs. In the end of the chapter, we outline some of the current state of the art methodology for computations of VCD spectra of large biopolymers.