We report a simple procedure to fabricate single crystals 3D C60 having an FCC structure on silicon substrates using a vapour–solid set-up in vacuum conditions. The morphology of the deposited film can be tuned by controlling the temperature and position of the substrate. The as-fabricated samples are extensively characterised by transmission electron microscopy, scanning electron microscope, X-ray powder diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy and nanoindentation, which allow us to shed light on the recrystallization process of the C60. In addition, the growth mechanism of the formation of crystalline 3D structure of the C60 film is discussed in detail. Based on the newly gained knowledge of mechanism and its unique properties, fullerene has shown huge potential as a solid lubricant on various kinds of substrates.