Dye-sensitized solar cells (DSSCs) are a promising third-generation photovoltaic cell technology whose advantages are low-cost fabrication, reduced energy payback time, better performance under diffuse light conditions and flexibility. Typically DSSCs employ toxic dyes such as metal-based porphyrins requiring complex synthesis. In contrast, natural pigments are environmentally and economically superior to synthetic dyes. However, narrow absorption spectra of natural pigments result in low efficiencies of the solar cells. Hence, co-sensitizing pigments with complementary absorption spectra, which increases the absorption band, is an attractive pathway to enhance the efficiency. In this paper, we report the performance of betanin-chlorophyll co-sensitized solar cell using betanin (λ max = 535 nm) and chlorophyll-a (λ max = 435 nm, 668 nm), natural pigments having complementary absorption spectra. Density functional theory simulations were performed to verify that the lowest unoccupied molecular orbital and the highest occupied molecular orbital levels of the dye molecules, are aligned appropriately with that of TiO 2 and the redox electrolyte, respectively, which is necessary for optimal device performance. Electrochemical impedance spectroscopic studies were performed to determine parameters corresponding to the charge transfer processes in the dye solar cells. Individual and co-sensitized solar cells were fabricated and the co-sensitized solar cell demonstrated a higher efficiency of 0.601% compared to efficiencies of 0.562% and 0.047% shown by betanin and chlorophyll solar cells, respectively.