Carbon microcoils were grown by the Ni-catalyzed pyrolysis of acetylene. The growth patterns and the tip morphologies of the carbon coils are examined in detail, and a growth mechanism is proposed. Basically, six thin fibers grew from a Ni catalyst grain during the initial growth stage immediately followed by the coalescence of the four fibers to form two fibers and then forming double-helixed carbon coils. A small amount of S and O, as well as C and Ni, was observed on the periphery of the cross section of the Ni catalyst grain. On the other hand, S and O were not observed in the central part. The driving force of the coiling of the straight fibers to form carbon coils is considered to be the strong anisotropy of the carbon deposition between different crystal faces.