Basic research is performed on the dependence of the composition, microstructure, topography, and nano-mechanical properties of ultra-thin carbon overcoats on plasma deposition conditions and the nano-tribological properties of these films. The processing parameters studied, based on a factorial design of experiments approach, are the RF power, chamber pressure, substrate bias voltage, and deposition rate. Correlations developed in this research lead to the identification of optimum film processing parameters and provide insight into micro-scale tribophenomena. The results help to enhance the technological basis for the design of anti-friction, wear-resistant interfaces of leading-edge technologies such as high-density magnetic recording.