The adsorption of 4-mercaptopyridine (4-Mpy) molecules on ZnS nanocrystals was investigated by means of Raman spectroscopy. We compared the Raman signals of 4-Mpy molecules adsorbed on ZnS nanocrystals and Ag substrate. The differences in the adsorption of 4-Mpy molecules on the semiconductor and the metal substrate were noted. The results demonstrated that adsorbed species on the semiconductor ZnS nanocrystals can be detected by Raman spectroscopy. Copyright © 2006 John Wiley & Sons, Ltd.