Adhesion layers are well-known to significantly improve the lifetime of MoS2-based solid lubricants. Typically, adhesion layers are “optimized” based on a phenomenological tests and then their deposition parameters are held fixed while the functional coating is studied. Here we examine the adhesion layer itself, while holding an MoS2 layer constant. In particular, the critical interfaces between the adhesion layer and the substrate, and between the adhesion layer and functional coating are regarded. MoS2-metal solid lubricant is chosen as the functional layer because it is a relatively brittle material whose performance is significantly affected by the quality and type of adhesion treatments. Substrate surface sputter cleaning was done by cathodic arc evaporation with different arc energies and substrate bias voltages. In addition to sputter etching of any surface oxides or other contaminants, some level of shallow implantation might be expected. The more usual surface preparation technique of argon plasma sputter etching was also used for comparison. Chromium and titanium were tested as adhesion layer materials. The adhesion layer thickness and deposition pressure were varied. Rutherford backscattering spectroscopy (RBS) and transmission electron microscopy (TEM) were used to analyze the adhesion layers and their interfaces with the substrates and with the MoS2-metal coatings. Ballon-disk tribometer sliding wear tests were made to assess changes in solid lubricant performance coming from variations in the adhesion layer. Scratch test characterizations were made to further evaluate adhesion layer performance.