Abstract: The geometries of a series of pushpull helicenes were optimized by using density functional theory B3LYP method at the 6-31G (d, p) basis set level. Based on the obtained stable molecular configuration, the frontier molecular orbits and electronic spectras of these molecules were calculated by using the ZINDO/SCI method. The results showed that the spatial molecular structures were different when the substituents or their positions were different.Through optimizing design, the distributions of HOMOs and LUMOs showed that these molecules have obviously charge transfer properties. Not only the nonlinear coefficients of this series of helicenes can be increased,but also the transparences of such molecules can be enhanced.