A fascinating nanoobject, possessing a hard core of multi-walled carbon nanotubes (MWNTs) and a relatively soft shell of brushlike polystyrene (PS) was chemically synthesized by thiol lactam initiated radical polymerization. FT-IR and X-ray photoelectron spectroscopy were employed to characterize the nanocomposites and electron microscopic methods were used to investigate the morphologies of the as-prepared hybrid nanocomposites. The MWNT-PS nanocomposites possess good dispersibility in common organic solvents. Transmission electron microscopic images of the samples provide direct evidence for the formation of a core-shell nanostructure, i.e., the MWNTs coated with the PS layer.