Single-wall carbon nanotubes (SWCNTs) and well-aligned thin multiwall carbon nanotubes (MWCNTs) were successfully synthesized via pyrolysis of a powder mixture of ferrocene and anthracene or 9,10-dibromoanthracene. It is shown that the size of the MWCNTs can be tuned just by changing the ratio of ferrocene/anthracene in the mixture. A lower ratio resulted in low-diameter MWCNTs containing up to five graphene layers only; a high ratio has led to thick MWCNTs with more than 25 layers. Furthermore, there are two extreme cases, the pyrolysis of powders at a low ratio of 1:7 that gives rise to carbon nanospheres and the pyrolysis of pure ferrocene in a H2 flow that mainly gives rise to metal nanoparticles. When powder mixtures of ferrocene and 9,10-dibromoanthracene are pyrolyzed, both SWCNTs and spherical carbon-coated iron nanoparticles are obtained.