The areal density of carbon nanotube forests can be increased up to the order of 1013 cm−2 using cycles of deposition and annealing of ultra-thin metal films, followed by nanoparticle immobilization. Herein, we show how the density of the catalyst nanoparticles increases after each cycle by using cross-sectional transmission electron microscopy. The layers of metal catalyst – subsequently deposited after previous annealing – sit on the uncovered areas of the support and, after annealing, restructure into nanoparticles cumulatively increasing the catalyst density. These nanoparticles lead to close-packed, high-density nanotube forests with nanotube areal densities of ∼1013 cm−2. The height of these high-density forests shortens as the density of the catalyst nanoparticle increases, which is observed using several synthesis conditions. This high nanotube density is required for using carbon nanotubes as interconnects in integrated circuits and in thermal interface materials.