In this study, we describe the growth mechanism and the ultralow friction and wear properties of smooth (20-50 nm rms) diamond films grown in a microwave plasma consisting of Ar and fullerene (the carbon source). The sliding friction coefficients of these films against Si{sub 3}N{sub 4} balls are 0.04 and 0.1 in dry N{sub 2} and air, which are comparable to that of natural diamond sliding against the same pin material, but is lower by factors of 5 to 10 than that afforded by rough diamond films grown in conventional H{sub 2}-CH{sub 4} plasmas. Furthermore, the smooth diamond films produced in this work afforded wear rates to Si{sub 3}N{sub 4} balls that were two to three orders of magnitude lower than those of H{sub 2}-CH{sub 4} grown films. Mechanistically, the ultralow friction and wear properties of the fullerene-derived diamond films correlate well with their initially smooth surface finish and their ability to polish even further during sliding. The wear tracks reach an ultrasmooth (3-6 nm rms) surface finish that results in very little abrasion and ploughing. The nanocrystalline microstructure and exceptionally pure sp{sup 3} bonding in these smooth diamond films were verified by numerous surface and structure analytical methods, including x-ray diffraction, high-resolution AF-S, EELS, NEXAFS, SEM, and TEM. An AFM instrument was used to characterize the topography of the films and rubbing surfaces