To fabricate flexible dye-sensitized solar cells (DSCs) utilizing full solar spectrum, the double-layered TiO2 films, selectively loading two different dyes in discrete layers, were formed on a plastic substrate by transferring the high-temperature-processed N719/TiO2 over an organic dye (TA-St-CA)-sensitized TiO2 film by a typical compression process at room temperature. It was found that interface control between two TiO2 layers is crucial for the efficient transport of photo-injected electrons from the N719/TiO2 to the TA-St-CA/TiO2 layer. Electron impedance spectra (EIS) and transient photoelectron spectroscopic analyses exhibited that introduction of a thin interfacial TiO2 layer between the two TiO2 layers remarkably decreased the resistance at the interface, while increasing the electron diffusion constant (Do) by 10 times. As a result, the photovoltaic conversion efficiency (eta) of the flexible tandem DSC was 6.64%, whereas that of the flexible cell derived from the single TA-St-CA/TiO2 layer was only 2.98%. Another organic dye (HC-acid), absorbing a short wavelength region of solar spectrum, was also applied to fabricate flexible tandem DSC. The 77 of the cell derived from the HC-acid/TiO2 layer was only 2.91%, but that of the tandem cell obtained by transferring the high-temperature-processed N719/TiO2 was 6.86%. (C) 2013 Elsevier Ltd. All rights reserved.