Poly-α-olefin (PAO) is an important synthetic fluid in the field of industry lubricants. To improve the tribological properties of PAO, a Schiff base copper complex was added to the lubricants. The tribological properties of steel and steel lubricated with PAO and PAOs containing a Schiff base copper complex were studied. The friction and wear properties of steel and steel lubricated with PAO and PAOs containing a Schiff base copper complex were evaluated using a SST-ST pin-disc tester. The sliding friction was measured using lubricants with or without a Schiff base copper complex and analyzed using surface analysis techniques including scanning electron microscopy, Fourier transform infrared spectroscopy, and confocal white light microscopy. A UMT-2 universal tribometer was also used to study the tribological properties of modifying PAO containing the Schiff base copper complex. The Schiff base copper complex structure was found to assist in the formation of a stronger tribofilm; more than the tribofilm prepared by lubricating only with PAO and this is crucial in obtaining a low and stable coefficient of friction. A lower stable friction coefficient and wear was found for the steel/steel surface contact when using the PAOs containing the Schiff base copper complex compared to the samples lubricated with the PAO without additives. The excellent tribological performance of the PAOs containing the Schiff base copper complex is attributed to the formation of a useful tribofilm with organic and inorganic groups on the sliding surface.