The crystallized free-standing through-hole TiO2 nanotube arrays (TNAs) membranes were fabricated by a facile method. CdS quantum dots (QDs) are assembled onto free-standing through-hole NTAs films using successive ionic layer adsorption and reaction (SILAR) process. The CdS/TNAs were easily transferred to the fluorine-doped tin oxide glass to form photoanodes after they were sensitized by modifying the traditional procedure. The morphology and crystalline phase of the TiO2 nanotubes were studied by field emission scanning electron microscopy (FESEM) and X-ray diffraction (XRD). The cells with 5 SILAR cycles show photovoltaic conversion efficiency as high as 3.34% under simulated sunlight (AM 1.5, 100 mW x cm(-2)). Obviously, the new approach promotes the uniform distribution of CdS on the densely aligned TNAs and prevents the clogging of CdS quantum dots (QDs) at the TiO2 nanotube mouth. Such enhanced properties may be ascribed to the strong combination between CdS and TiO2, favorable for charge separation of TNAs.