The carbon micro-coils were obtained by the Ni-catalyzed pyrolysis of acetylene. The carbon micro-coils with various coiling morphology: regular double coils, coils built up by circular or flat fibers, super helix coils, single coils, etc. can be observed. The carbon coils with various coil diameters and coil pitches were obtained by controlling reaction conditions, such as reaction temperature, source gas flow rate of sulfur-impurity, acetylene or hydrogen.