In the present work, TiO2 nanoparticle and multi-walled carbon nanotubes composite powder is prepared hydrothermally. After doctor blading the paste from composite powder, the resulted composite film is sensitized with Cu-based metal-organic frameworks using a layer-by-layer deposition technique and the film is characterized using FE-SEM, EDX, XRD, UV/Visible spectrophotometry and photoluminescence spectroscopy. The influence of the carbon nanotubes in photovoltaic performance is studied by constructing a Grätzel cell with I3(-)/I(-) redox couple containing electrolyte. The results demonstrate that the introduction of carbon nanotubes accelerates the electron transfer, and thereby enhances the photovoltaic performance of the cell with a nearly 60% increment in power conversion efficiency.