The controlled preparation of two-dimensional (2D) and three-dimensional (3D) dendritic nanostructures of CdS was reported. 2D dendritic patterns are obtained through the self-assembly of nanoparticles under the entropy-driven force. 3D dendritic needle-like nanocrystals are prepared through an aqueous solution synthesis regulated by oleic acid molecules. Their growth mechanism is presumed to be the selective binding of OA molecules onto growing crystal planes. Techniques such as SEM, TEM, XRD, and FT-IR were employed to characterize the morphologies and structures of the obtained products.