Novel sp3 rich diamond-like carbon (DLC) nanorod films were fabricated by hot filament chemical vapor deposition technique. The results are indicative of a bottom-up self-assembly synthesis process, which results in a hierarchical structure that consists of microscale papillae comprising numerous nanorods. The papillae have diameters ranging from 2 to 4 μm and the nanorods have diameters in the 35-45 nm range. A growth mechanism based on the vapor liquid-solid mechanism is proposed that accounts for the morphological aspects in the micro- and nano-scales.