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Selective growth of vertically aligned and highly dense carbon nanotubes was achieved by using thermal chemical vapor deposition via careful selection of a thin catalyst layer and an appropriate supporting layer. It was found that carbon nanotube growth was significantly enhanced when tantalum was used as the supporting layer on which a thin iron catalyst was deposited. Cross-sectional transmission electron microscopy revealed a Stranski-Krastanov mode of iron island growth on tantalum with relatively small contact angles controlled by the relative surface energies of the supporting layer, the catalyst, and their interface. The as-formed iron island morphology promoted vertical growth of carbon nanotubes.