Conventional magnetron discharge is a widely used technology for many applications. In the last decade, the high current density sputtering regime has been an interesting alternative for tailoring thin film properties. In this paper, we focused on the electrical characterization of the helium magnetron plasma operated at average gas pressure (5 Pa) with a molybdenum target. Optical emission spectroscopy diagnostics also supports this study by providing information on electron density evolution. The analysis of the plasma–surface interaction zone on the target unveiled the physical mechanisms associated with the high current density range (6 A cm−2), corresponding to different discharge regimes. The self-sputtering yield plays a key role in high-power impulse magnetron sputtering discharge operated with helium. The electron density is highly dependent on the presence of a metal.