Micro-coiled carbon fibers were directly prepared on the graphite substrate using co-electrodeposition of nickel and sulfur as catalysts, in this paper. The diameter of coil and that of micro-coiled carbon fiber are about 800 nm and 400 nm, respectively. Compared with the current preparation methods of catalysts, electrochemical deposition is an effective, cheap and simple technique. Especially, this method is suitable for preparation of ally catalyst. The parameters of electrochemical deposition (deposition time and current density) have little influence on helix of growth and growth mechanis...