Communication: The influence of chirality on the nonlinear optical properties of poly(isocyanide)s is examined. It is found that the chiral and nonlinear properties can occur on different levels of the molecular structure and can therefore be separately tuned, but that they still can be coupled together. The NLO properties of chiral molecules can also be enhanced significantly by optimizing the magnetic contributions to the nonlinearity, an important result for applications in electro-optics.