A sonication-assisted sequential chemical bath deposition (S-CBD) approach is presented to uniformly decorate CdS quantum dots (QDs) on self-organized TiO2 nanotube arrays (TNTAs). This approach avoids the clogging of CdS QDs at the TiO2 nanotube mouth and promotes the deposition of CdS QDs into the nanotubes as well as on the tube walls. The photoelectrochemical and photocatalytic properties of the resulting CdS-decorated TNTAs were explored in detail. In comparison with a classical S-CBD approach, the sonication-assisted technique showed much enhancement in the photoelectrochemical and photocatalytic activities of the CdS QDs-sensitized TNTAs.