The present work represents successful synthesis of CdTe-sensitized TiO 2 nanoarray thin films by two simple chemical routes. Here, we report the sensitization of TiO 2 nanoarrays with CdTe nanoparticles through the electrodeposition technique at ambient condition. The electrodeposition of 30 min leads to the formation of shell of CdTe nanoparticles over TiO 2 nanoarrays. This core-shell formation structure was further confirmed by TEM and HR-TEM analysis. Optical absorption and photoelectrochemical study revealed that the TiO 2 /CdTe core-shell heterostructure extend the absorption edge of titania in the visible region of solar spectrum; it also facilitates the efficient charge transport and reduces the recombination losses. The maximum photoconversion efficiency of 0.32% is obtained for TiO 2 /CdTe core-shell semiconductor-sensitized solar cells (SSSCs).