The effect of compositions of Al2O3 in the mixed Fe/Al2O3 catalysts on the synthetic behaviors of carbon nanotubes (CNTs) by catalytic chemical vapor deposition (CCVD) process was investigated in wide range of the mixture ratios of support materials. CNTs were synthesized with Fe/Al2O3 catalysis under the condition of 40 min in synthetic time, and 923 K of synthetic temperature using C2H4 and H2 as synthetic and carrier gas, respectively. The carbon yield with the content of Al2O3 showed in a parabolic curve and the maximum carbon yield was 40 wt.% of Al2O3. As the mixture ratio of Al2O3 increased, decreasing tendency was observed in the diameter of CNTs. Specific surface areas of CNTs were increased with the increase of the mixture ratio of Al2O3.