Controllable synthesis of one-dimensional (1D)/three dimensional (3D) nanocomposites with promising photocatalytic performances has been attracting ever-increasing research attention in recent years. Here, we report the self-assembly of TiO2 nanobelts/CdS nanospheres (TNBs/CdS NSPs) photocatalyst via the electrostatic interaction of positively charged CdS nanospheres (CdS NSPs) with negatively charged TiO2 nanobelts in aqueous phase. The as-formed TNBs/CdS NSPs nanocomposite exhibited significantly enhanced visible-light-driven photocatalytic activities in comparison with the single counterpart (TNBs and CdS NSPs) owing to the formation of well-defined-heterojunction between TNBs and CdS NSPs, thus leading to much enhanced light absorption and prolonged lifetime of photogenerated charge carriers. It is anticipated that our work could provide an efficient synthetic approach to design a large variety of 1D/3D photocatalysts for diverse photocatalytic applications. (C) 2015 Elsevier B.V. All rights reserved.