The potential of organic electro-optic materials for large electro-optic activity and fast response to applied electric fields (leading to 100 GHz device bandwidths) is important and increasingly well-recognized. In this communication, we demonstrate how quantum and statistical mechanical calculations can be used to guide the systematic improvement of both molecular first hyperpolarizability (β) and macroscopic electro-optic activity (r). Femtosecond time-resolved, wavelength-agile Hyper-Rayleigh Scattering (HRS) measurements have been used to measure β values relative to chloroform and to avoid confusion associated with two photon contributions. Electro-optic coefficients have been characterized by simple reflection (Teng-Man method), attenuated total reflection (ATR), and Mach Zehnder interferometry. "Constant bias" modifications of these techniques have been used to permit investigation of optimized poling conditions. Organic electro-optic materials also afford unique advantages for the fabrication of conformal and flexible devices, for the integration of disparate materials, and for exploitation of novel manufacturing technologies such as soft lithography. Both stripline and ring microresonator structures have been fabricated by soft lithography. The integration of organic electro-optic materials with silicon photonics (both split ring microresonators and photonic bandgap circuitry) has been demonstrated.