Morphology-controllable carbon nanocoils (CNCs) are synthesized by thermal chemical vapor deposition using Ni nanoparticle as catalyst prepared by spray-coating method. It is found that, with the increase of number of spray-coating times, the helicity of CNCs increases whereas the average line diameter and coil pitch decrease. Additionally, infrequent Y-junction CNCs and plait-like CNCs are found in the deposits. What is noteworthy is that, compared with dip-coating, spray-coating method can prepare more uniform catalyst on substrate, resulting in more CNCs with high purity.