This study investigates the sliding wear behaviour of amorphous carbon (a-C) and tetrahedral amorphous carbon (ta-C) coatings, two forms of diamond-like carbon (DLC) coatings, against SAE 52100 steel using a modified ball-on-disk tribometer with applied electrical currents ranging from 100 mA to 1800 mA. It focuses on the variations in sliding friction and wear characteristics of these coatings as electrical currents increase under constant load and speed conditions. The a-C coatings exhibited lower coefficient of friction (COF) values and reduced volumetric wear losses up to 1500 mA, while ta-C coatings studied displayed higher wear, similar to uncoated M2 steel, at 300 mA with degradation occurring at low currents, resulting in failure due to severe oxidational wear. The a-C coatings showed no significant electrical damage at these currents. Raman spectroscopy revealed structural changes on the wear tracks of sp2-rich a-C coatings, specifically the formation of graphene layers. In comparison, the wear tracks of sp3-rich ta-C coatings did not display such transformation under the conditions studied. The graphene coverage on the surfaces of the a-C coatings increased with the increase in the current as revealed by the Raman intensity maps of 2D peaks and this increase was accompanied by a higher defect density in the graphene. The low COF of graphene-covered a-C surfaces was consistent with the proposed mechanisms of moisture adsorption. However, at currents exceeding 900 mA, surface temperatures of a-C coatings exceeded 100 °C, impairing graphene’s ability to maintain low friction, resulting in an increased COF.