We explored advantages of diverse carbon nanotube forests with tailored structures synthesized by water-assisted chemical vapor deposition (CVD) growth (supergrowth) from engineered catalysts. By controlling the catalyst film thickness, we synthesized carbon nanotube (CNT) forests composed from nanotubes with different size and wall number. With extensive characterizations, many interesting dependencies among CNT forest structures and their properties, which were unknown previously, were found. For example, multiwalled carbon nanotubes (MWNTs) showed superior electronic conductivity while single-walled carbon nanotubes (SWNTs) showed superior thermal diffusivity, and sparse MWNTs achieved lower threshold voltage for field emission than dense SWNTs. These interesting trends highlight the complexity in designing and choosing the optimum CNT forest for use in applications.