Zinc sulfide (ZnS) nanocrystals with graphite sheaths were obtained from pyrolysis of bis(2-mercaptobenzothiazolato)-zinc (II) in nitrogen atmosphere at 400°C for 2 h without any additional sources. X-ray diffraction patterns showed that the ZnS crystals belonged to the hexagonal system. Transmission electron microscope studies revealed that ZnS/C nanocrystals were well-dispersed and had a diameter of 20~30 nm. The possible mechanism for the formation of the interesting well-dispersed microstructures was also proposed.The special structures of ZnS nanocrystals with graphite sheaths may have potential applications in nanoelectronics and photonics. This simple approach may be applied to the synthesis of other semi-conductor nanocrystals.