The core-shell CdS-carbon (CdS/C) nanoparticles were synthesized for the first time via a facile pyrolysis approach of bis(beta-mercaptoethanol)-cadmium(II) as a single-source precursor. After using acid treatment method, well-dispersed and homogeneous core-shell CdS/C nanoparticles were obtained. The morphology, structure, and properties of CdS/C nanoparticles were investigated by X-ray diffraction (XRD), Raman spectra, transmission electron microscopy, X-ray photoelectron spectroscopy (XPS), and fluorescence spectroscopy. Most of the prepared nanoparticles presented core-shell structures with core diameter of similar to 10 nm and shell thickness of similar to 4 nm. The CdS core belonged to hexagonal crystal system. The carbon shell was employed as a good dispersion medium to form well-dispersed small sized CdS particles. XRD and XPS results revealed that there is an interaction between CdS core and carbon shell. Fluorescence measurement showed that the monodispersed CdS-carbon nanoparticles exhibit remarkable fluorescence enhancement effect compared with that of the pristine CdS nanoparticles, which indicates the prepared nanoparticles are a promising photoresponsive material.