Second-order nonlinear optics (NLO) requires materials that are noncentrosymmetric on a molecular and macroscopic scale. Usually such materials are designed by incorporating noncentrosymmetric chromophores into a noncentrosymmetric macroscopic structure such as poled polymer films, Langmuir Blodgett films, or crystals. The nonlinear optical properties can be improved by optimizing the molecular NLO response or the alignment of the chromophores in the macroscopic structure. In this paper, we demonstrate a new approach to optimize the NLO properties of a material by using supramolecular aggregation and chirality.