Achieving a significant friction reduction is crucial for using thermoplastic materials as substrates in tribological applications and presents an eligible alternative to the use of light metals. In this study, previously developed MoS2/graphite/zinc composite coatings, applied by an atmospheric pressure plasma deposition (APPD) process, were investigated to extend the understanding of their characteristics and the influence of the process and environmental parameters on friction behavior. Tribological tests were conducted in ambient conditions and at elevated temperatures (110 °C) to study the friction behavior under application-oriented conditions. The presence of atmospheric oxygen during the deposition process was shown to influence the durability of the coatings, which motivated the application of an inert gas atmosphere for the coating deposition. A novel shrouding plasma nozzle was introduced, which further lowered the friction coefficients. The oxidizing effect of the plasma spray deposition was studied with X-ray photoelectron spectroscopy to investigate the strong impact of the deposition current on the friction behavior and durability of the deposited coatings. Coating composition, morphology, and the effects of the tribological testing were evaluated using optical microscopy, 3D surface measurements, scanning electron microscopy, X-ray diffraction, and nanoindentation. The fabricated coatings with thicknesses in the 10 μm range and good adhesion on the polyamide substrate were stable under extended testing durations and at elevated temperatures and accomplished a significant friction reduction compared to the uncoated polyamide. Thus, APPD-fabricated MoS2/graphite/zinc coatings represent an excellent candidate for low-friction applications of thermoplastic substrates.