We characterize the photorefractive behavior of a photorefractive multicomponent polymer composite of PVK-TCP:C60:DEANST. Efficient plasticization of the host polymeric matrix and utilization of a nonlinear chromophore with a large dipole moment provide a large poling-induced electro-optic coefficient. Diffraction efficiencies as high as 40% and asymmetric net two-beam coupling gain coefficients in excess of 130 cm−1, surpassing those of known inorganic single-crystalline photorefractive media, are reported.