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A method to synthesize high-density, vertically-aligned, multi-wall carbon nanotubes (MWCNTs) on an insulating substrate at low temperature using a complementary metal–oxide–semiconductor (CMOS) compatible process is presented. Two factors are identified to be important in the carbon nanotube (CNT) growth, which are the catalyst design and the substrate material. By using a Ni–Al–Ni multilayer catalyst film and a ZrO2 substrate, vertically-aligned CNTs can be synthesized at 340 °C using plasma-enhanced chemical vapor deposition (PECVD). Both the quality and density of the CNTs can be enhanced by increasing the synthesis temperature. The function of the aluminum interlayer in reducing the activation energy of the CNT formation is studied. The nanoparticle sintering and quick accumulation of amorphous carbon covering the catalyst can prematurely stop CNT synthesis. Both effects can be suppressed by using a substrate with a high surface energy such as ZrO2. [ABSTRACT FROM AUTHOR]