The concept for inorganic-organic device is an attractive technology to develop devices with better characteristics and functionality due to the complementary advantages of inorganic and organic materials. This chapter provides an overview of the principal requirements for organic and inorganic semiconductor properties and their fabrication processes and focus on the compatibility between low temperature plasma enhanced chemical vapor deposition (PECVD) and polymer organic materials deposition. The concept for inorganic-organic device was validated with the fabrication of three hybrid thin film photovoltaic structures, based on hydrogenated silicon (Si:H), organic poly(3-hexythiophene): methano-fullerenephenyl-C61-butyric-acid-methyl-ester (P3HT:PCBM), and poly(3,4 ethylenedioxythiophene): poly(4-styrenesulfonate) (PEDOT:PSS) films. Optoelectronic characteristics, performance characteristics, and interfaces of the different configurations aspects are discussed. Hybrid ITO/PEDOT:PSS/(i)Si:H/(n)Si:H structure results in a remarkably high short circuit current density as large as 17.74 mA/cm 2 , which is higher than the values in organic or inorganic reference samples. Although some hybrid structures demonstrated substantial improvement of performance, other hybrid structures showed poor performance, further R&D efforts seem to be promising, and should be focused on deeper study of organic materials and related interface properties.