This work determines the effect of compact TiO2 layers that are deposited onto fluorine-doped tin oxide (FTO), to improve the performance of dye-sensitized solar cells (DSSC). A series of compact TiO2 layers are prepared using radio frequency (rf) reactive magnetron sputtering. The films are characterized using X-ray diffraction (XRD), atomic force microscopy (AFM), scanning electron microscopy (SEM), and UV-Vis spectroscopy. The results show that when the Ar/O2/N2 flow rates are 36 : 18 : 9, the photo-induced decomposition of methylene blue and photo-induced hydrophilicity are enhanced. After annealing at 450°C in an atmosphere ambient for 30 min, the compact TiO2 layers exhibit higher optical transmittance. The XRD patterns for the TiO2 films for FTO/glass show a good crystalline structure and anatase (101) diffraction peaks, which demonstrate a higher crystallinity than the ITO/glass films. As a result of this increase in the short circuit photocurrent density, the open-circuit photovoltage, and the fill factor, the DSSC with the FTO/glass and Pt counter electrode demonstrates a solar conversion efficiency of 7.65%.