Understanding the tribological basics is essential to extending the service life of machine elements and lubricants. For this purpose, it is necessary to study the micro-/nanotribological interactions between the lubricant and the macro-structure's surface , , . This paper deals with the influence of lubricating grease composition, in particular the presence of antioxidants, on the grease service life and the tribological performance characteristics of boundary layers in high-speed ball bearings. First of all, the experimental set-up including the bearing test rig, the test parameters and the six model greases will be presented. Thereafter, the equipment for measuring the nanomechanical properties of the boundary layers and the metal surfaces will be described. Experimental results from tribophysical tests like nanohardness measurements and nanoscratch tests include information about the structure of the boundary layers. Finally, these results will be correlated with grease and boundary layer chemical composition as well as with grease service life.