We report a rapid and low temperature process for fabricating composite TiO2 electrodes for dye-sensitized solar cells on glass and plastics by in tandem spray deposition and laser annealing. A homogenized KrF excimer laser beam (248 nm) was used to layer-by-layer anneal spray deposited TiO2 nanoparticles. The produced TiO2 film is crack free and contains small particles (30 nm) mixed with different fractions of larger particles (100–200 nm) controlled by the applied laser fluence. Laser annealed double-layered structure is demonstrated for both doctor-blade deposited and spray-deposited electrodes and performance enhancement can be observed. The highest demonstrated all-laser-annealed cells utilizing ruthenium dye and liquid electrolyte showed power conversion efficiency of ∼3.8% under simulated illumination of 100 mW/cm2.