The creation of nanoscale organic–inorganic hybrid coatings with uniform architecture and high surface area, while maintaining their structural and morphological integrity, remains a significant challenge in the field. In this study, we present a novel solution, by utilizing Atomic/Molecular Layer Deposition (ALD/MLD) to coat patterned vertically aligned carbon nanotube micropillars with a conformal amorphous layer of Fe-NH2TP, which is a trivalent iron complex complexed with 2-amino terephthalate. The effectiveness of the coating is verified through multiple analytical techniques, including high-resolution transmission electron microscopy, scanning transmission electron microscopy, grazing incidence X-ray diffraction, and Fourier transform infrared spectroscopy. The Fe-NH2TP hybrid film exhibits hydrophobic properties, as confirmed by water contact angle measurements. Our findings contribute to advancing the understanding of how to grow high-quality one-dimensional materials using ALD/MLD and hold promise for future research in this area.