Under the high-contact-pressure and shear conditions of tribological interfaces lubricated by gaseous, liquid, and solid forms of carbon precursors, a variety of highly favorable tribocatalytic processes may take place and result in the in situ formation of nanocarbon-based tribofilms providing ultralow friction and wear even under extreme test conditions. Structurally, these tribofilms are rather complex and may consist of all known forms of nanocarbon including amorphous or disordered carbon, graphite, graphene, nano-onion, nanotube, etc. Tribologically, they shear readily to provide ultralow friction and protection against wear. In this paper, we review some of the latest developments in catalyst-enabled tribochemical films resulting from gaseous, liquid, and solid sources of carbon. Particular focus is given to the nature and lubrication mechanisms of such in situ derived tribofilms with the hope that future tribological surfaces can be designed in such a way to exploit the beneficial impact of catalysis in friction and wear control.