TiO2 nanotube arrays sensitized by PbS nanoparticles (TiO2 NTs/PbS) with enhanced visible-light activity were synthesized by a two-step approach including an electrochemical anodization technique followed by an in situ photodeposition approach. The structural investigations indicated that PbS nanoparticles grew uniformly on the walls of the TiO2 NTs. The TiO2 NTs/PbS exhibited more excellent photoelectrochemical properties than that of the TiO2 NTs under visible-light irradiation. The enhanced photoelectrochemical activity of the TiO2 NTs/PbS could be attributed to the improvement of visible-light absorption and charge separation derived from the coupling effect of the PbS nanoparticles and TiO2 NTs.