We demonstrate a unique single-pot synthesis of self-organized structures of CdS/dendrimer nanocomposites having long-range correlation by adopting a radiation-induced technique. The present method has been able to produce long-range chain-like networks of CdS nanoparticles of high stability within the dendrimer matrix with particle size monodispersity ∼6%, as visualized with atomic force microscopy, while individual particles are characterized by transmission electron microscopy, photoluminescence, absorption spectroscopy and dynamic light scattering. Results point to a possible mechanism of long-range self-organization from the nanometer to micrometer length scales, where the self-organization is controlled by surface functionality of the dendrimer molecule, solvent and crystal phase of the CdS nanocrystals. The present investigation opens up new potential routes to manipulate semiconductor nanocomposites for optical diagnostics and for applications that require dendrimer nanocomposites with a long-range order.