We investigated how changes in the method of supplying Sn and Fe carbon nanocoil (CNC) catalysts affected the results of chemical vapor deposition. The Sn/Fe catalysts were supplied using the following four materials: a thin Sn film, a drop-coated solution of Fe2O3, tetramethyltin (TMT) vapor, and ferrocene vapor. The CNC purity was evaluated using scanning electron microscopy. The CNC purity in the overall carbon deposit was also evaluated by analyzing the cross-section of the deposit. The CNC purity averaged over the overall carbon deposit was increased 1.5-fold by the TMT supply. We obtained a maximum CNC purity of 72% using a combination of TMT and ferrocene vapors, with Sn/Fe deposition on the substrate. Energy-dispersive x-ray spectroscopy analysis of the catalyst nanoparticles in the tips of the CNCs and carbon nanofibers (CNFs) revealed that there was a large difference in the Sn/Fe molar ratios for the angular- and round-type CNFs.