Hydrothermal strategies were successfully used to control the phases and morphologies of CdS nanocrystals. In the absence of an external direction-controlling process, the hexagonal and cubic phase well-defined leaf- and flower-like CdS nanocrystals were controlled obtained via adjusting the reaction duration or the concentration of surfactant. Oriented attachment growth modes were suggested for the formation of CdS superstructures, which was clarified through the tracing of temporal evolution of CdS nanoparticles. The CdS superstructures were structured by primary building nanoparticles, and held excellent visible emission with a peak in the green regions. This strategy is very helpful for studying the phase and morphology controlled fabrication of sulfides nanocrystals. (C) 2012 Elsevier B.V. All rights reserved.