Vacuum and air atmospheres impose very different requirements on tribological-loaded contacts, which usually require different surface materials. While hard tetrahedral amorphous carbon (ta-C) coatings provide good tribological properties in air, soft coatings such as molybdenum disulfide (MoS2) work well in a vacuum. Tribological performance in the respective other environment, however, is poor. In this work, the combination of laser microstructured (direct laser interference patterning) steel substrates and the deposition of ta-C and MoSx coatings with vacuum arc evaporation (LaserArc™) was studied, resulting in steel/DLIP, steel/DLIP/ta-C, steel/DLIP/MoSx, steel/DLIP/ta-C/MoSx, and steel/MoSx surface combinations. The tribological properties were studied using a ball-on-disk tribometer with a steel ball counter body in air and in a vacuum (p < 5 × 10⁻⁷ mbar). The type of the topmost coating governed their tribological properties in the respective atmosphere, and no general beneficial influence of the microstructure was found. However, steel/DLIP/ta-C/MoSx performed best in both conditions and endured the highest contact pressure, which is attributed to the mechanical support of the ta-C coating and MoSx reservoir in the remaining structure, as evidenced by Raman spectroscopy. The findings suggest that such combination allows for surfaces bearing a high load capacity that can be applied in both a vacuum and in air, for example, in multi-use space applications.