The investigation of the use of cyanine dyes in thin-film heterojunction photovoltaic devices was reported. It was shown that a carbocyanine dye acts as donor in conjunction with buckminsterfullerene (C60). Cyanine acts as acceptor when copoly(dicyano-phenylvinylene-triphenylamine) is used as donor. It was concluded that the electron energy levels of the frontier orbitals of the dye allow it to be used as donor and acceptor at the same time.