Herein we report our recent efforts in employing natural materials and synthetic derivatives of natural molecules for organic field effect transistors (OFETs) and organic photovoltaics (OPVs). We evaluated dyes from the following chemical families: acridones, anthraquinones, carotenoids, and indigoids. These materials have proven effective in organic field effect transistors, with mobilities in the 4 × 10-4 - 0.2 cm2/V-s range, with indigoids showing promising ambipolar behavior. We fabricated complementary-like voltage inverters with high gains using indigoids. The photovoltaic properties of these materials were characterized in metal-insulator-metal (MIM) diodes, as well as in donoracceptor bilayer devices. Additionally, we have found that indigoids and Quinacridone, show long-range crystalline order due to hydrogen binding, and have considerably higher relative permittivities (ε) compared to typical organic semiconductors. Higher permittivities result in lower exciton binding energies and thus may lead to high photocurrents in photovoltaic devices.© (2011) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.