The co-sensitization of two organic dyes (SQ1 and JK2), which are complementary in their spectral responses, shows enhanced photovoltaic performance compared with that of an individual organic dye-sensitized solar cell. The power conversion efficiency of the co-sensitized organic dye solar cell based on the newly developed binary ionic liquid (solvent-free) electrolyte gives 6.4% under AM 1.5 sunlight at 100 mW/cm2 irradiation, which is higher than that of individual dye-sensitized solar cells. The incident monochromatic photon-to-current conversion efficiency (IPCE) of the co-sensitized solar cell shows typical absorption peaks at 530 and 650 nm corresponding to the two dyes and displays a broad spectral response over the entire visible spectrum with IPCE of >40% in the 400-700 nm wavelength domain.