The plasmonic effects of infiltrated silver (Ag) nanoparticles, with different contents, inside a nanostructured TiO2 film on the photovoltaic performance of dye-sensitized solar cells (DSSCs) are explored. The synthesized Ag nanoparticles are immobilized onto deposited TiO2 nanoparticles by a new strategy using 3-mercaptopropionic acid (MPA), a bifunctional linker molecule. Transmission electron microscope (TEM) images show that monodispersed Ag and polydispersed TiO2 nanoparticles have an average diameter of 12 ± 3 nm and 5 ± 1 nm, respectively. Moreover, Fourier transform infrared spectroscopy (FTIR) analysis reveals that Ag nanoparticles were successfully functionalized and capped with MPA. Optical studies on the MPA-capped Ag nanoparticles inside TiO2 film show an increase in the total absorbance of the electrode. Moreover, EIS measurements confirm that MPA-capped Ag nanoparticles inhibit the charge recombination and improve the stability of nanoparticles in I3-/I- electrolyte. The DSSC assembled with optimal content of MPA-capped Ag nanoparticles demonstrated an enhanced power conversion efficiency (8.82% ± 0.07%) compared with the pure TiO2 (7.30% ± 0.05%). The increase in cell efficiency was attributed to the enhanced dye light absorption in strength and spectral range due to the surface plasmon resonance of MPA-capped Ag nanoparticles in the photoanode.