The interaction between the main operational variables during the growth of vertically aligned multiwalled carbon nanotubes (VA-MWCNTs) by catalytic chemical vapor deposition is studied. In this contribution, we report the influence of the carbon source (i.e. acetylene, ethylene and propylene), the reaction/activation temperature, the rate of heating, the reaction time, the metal loading, and the metallic nanoparticle size and distribution on the growth and alignment of carbon nanotubes. Fe/Al thin films deposited onto silicon samples by electron-beam evaporation are used as catalyst. A phenomenological growth mechanism is proposed to explain the interaction between these multiple factors. Three different outcomes of the synthesis process are found: i) formation of forests of non-aligned, randomly oriented multi-walled carbon nanotubes, ii) growth of vertically aligned tubes with a thin and homogeneous carbonaceous layer on the top, and iii) formation of vertically aligned carbon nanotubes. This carbonaceous layer (ii) has not been reported before. The main requirements to promote vertically aligned carbon nanotube growth are determined.