From the moment of conductive polyacetylene discovery, semiconducting polymers and other organic thin films and multilayers are important for a wide range of applications, including electronics, photovoltaics and sensors. The main idea of this chapter is the synthesis of new conjugated donor and acceptor polymers and development of organic solar cells on their basis. As donor polymers were used modified polyanilines (PANIs) and its dopants, as acceptor compounds-the fullerene C 60 derivatives. Experimental prototypes of organic solar cells were obtained on the basis of binary donor-acceptor layers and bulk heterojunctions, consisting of novel polyaniline derivatives and fullerene-contained polymers. The current-voltage characteristics of solar cells were measured and the values of such parameters, such as open-circuit voltage, short-circuit current, fill factor and power conversion efficiency, were calculated. Comparison of parameters of the various types of organic solar cells was held.