The use of tungsten disulfide in tribofilms on functional surfaces has been a proven way to reduce the frictional losses in rolling and sliding contacts, especially in lubricated contacts at boundary and mixed regime. A suitable and cost-effective process to deposit tungsten disulfide is by ANS Triboconditioning, the mechano-chemical surface finishing process for improving the tribological properties of mechanical components made of steel or cast iron. However, it is not known what are the optimal process parameters, speeds and pressures, to achieve an optimal surface treatment. In this paper, the modifications of the work-piece surfaces under Triboconditioning have been tracked to optimize the process parameters. To closely control the conditions, a commercial tribometer with a block-on-ring configuration was used. Cylindrical tungsten carbide samples (representing the tool) were rubbed against steel rings (representing the work-piece) under two different loads and speeds. The ring surfaces of two different finishes (ground and honed) were measured on the same place before and after treatment to track the surface modifications. At last, the treated rings were rubbed against a flat steel surface in start-stop sequences that resemble pin-roller operating conditions of a truck valve train and the friction behavior was screened. The results show a reduction of the core roughness of the ring surfaces with the lowest friction for the ground rings treated by low load and low speed.