The emergence of vegetable oil as a promising alternative lubricant in the tribological application space has fueled research for making these oils as useful as mineral oils. Tribological modification of vegetable oil by the addition of TiO2/gC3N4 nanocomposite (as a nanoadditive) was studied here. The dispersion of the nanoadditive in the vegetable oil showed good oil dispersion stability without the addition of any surfactant. The tribological studies were conducted in a four-ball tester using ASTM standard D5183. In addition, the effect of temperature on tribological performance was also studied to understand the oxidation behavior of vegetable oil. The results showed a significant improvement in friction and wear properties of the optimized nano-oil. The mechanism behind the improvement in friction and wear properties is annotated in this paper.