We report an enhancement of photovoltaic response by dispersing phosphorescent dye fac tris (2-phenylpyridine) iridium (Ir(ppy)3) in organic solar cells of poly[2-methoxy-5-(2¡¦-ethylhexyloxy)-1,4-phenylenevinylene] (MEH-PPV) doped with surface-functionalized fullerene 1-(3-methyloxycarbonyl)propy(1-phenyl [6,6] C61 (PCBM). It is known that photoexcitation generates both singlet and triplet states through intersystem crossing caused by hyperfine or spin-orbital coupling. Due to long diffusion length the triplet excitons can migrate from their generation sites to the interfaces of donor-acceptor interaction and directly dissociate into charge carriers. We found, based on the studies of magnetic field-dependent photocurrent, that the dispersed Ir(ppy)3 molecules increase the spin-orbital coupling strength and triplet density in the MEH-PPV matrix due to the penetration of MEH-PPV π electrons into the large field of orbital dipoles of the Ir(ppy)3. Especially, the triplet excitons facilitate the direct dissociation into charge carriers at the donor-acceptor interacting interfaces in the composite of MEH-PPV and PCBM, and consequently improve the photovoltaic response in organic solar cells.