Our research in nonlinear optic (NLO) polymer-based electro-optic (EO) modulators has centered on optimizing device performance through the using of polymer cladding layers with higher relative conductivities than the NLO core material. We have demonstrated as much as a 10 times increase in the effective EO coefficient of electrode poled, guest/host NLO polymers, compared to using passive polymer claddings. We have achieved the lowest poling voltage to date for maximum EO coefficient, 300 V, for a two-layer waveguide structure consisting of a 2 µm thick NLO polymer layer and 2 µm thick conductive cladding layer. Optimized polymer cladding materials posessing the desired optical and electromagnetic properties we find need to be balanced with materials processability. In addition to the conventional polymer materials under investigation, a novel material, deoxyribonucleic acid (DNA), derived from salmon sperm, has shown promise in providing both the desired optical and electromagnetic properties, as well as the desired resistance to various solvents used for NLO polymer device fabrication. Our investigation also includes intercalation of fluorescent dyes, photochromic dyes, nonlinear optic chromophores, two-photon dyes, and rare earth compounds into a DNAbased host material and comparing results with poly(methyl methacrylate) (PMMA)-based host materials.