We explored new strategies for efficiency enhancement in dye-sensitized solar cells (DSSCs) by combining dehydration–condensation reactions with sputtering deposition methods. The photoanodes were realized by means of low-temperature preparation of mesoporous TiO2 films on thin undoped TiO2 compact (blocking) layers on ZnO:Al (AZO) substrates and sensitization with ruthenium dye, N719. For photoanodes fabrication, an 8 μm thick mesoporous film of TiO2 and an under critical thermal budget, applied before dye loading (≤200 °C: i.e., 150 °C for the TiO2 mesoscopic layer and 200 °C for the TiO2 blocking/AZO bilayer), were employed, which renders the overall process competitive for the applications. The structural properties of the sputtered TiO2/AZO bilayer were optimized, and a cell efficiency as high as the 4.6%, above the current literature limit for AZO-based DSSC (3.8% for 10 μm thick …