This novel scientific development introduces a new method and new materials to produce multilayered, nonlinear optical films. Potential applications include electro-optic modulators and frequency doubling devices. The materials and processing steps used result in high degree of non-centrosymmetry in the film, thus forming high net polar ordering which is very useful for various electro-optical applications. Compared to existing electro-optic modulators, this innovation offers advantages, including, higher nonlinear susceptibilities, high modulation rates, and lower device fabrication costs.