Aluminum is widely used in electrical contacts due to its electrical properties and inexpensiveness when compared to copper. In this study, we investigate the influence of operating conditions like contact load (pressure), sliding speed, current, and surface roughness on the electrical and tribological behavior of the interface. The tests are conducted on a linear, pin-on-flat tribo-simulator specially designed to investigate electrical contacts under high contact pressures and high current densities. Control parameters include sliding speed, load, current, and surface roughness. The response of the interface is evaluated in the light of coefficient of friction, contact resistance, contact voltage, mass loss of pins, and interfacial temperature rise. As compared to sliding speed, load, and roughness, current is found to have the greatest influence on the various measured parameters. Under certain test conditions, the interface operates in a “voltage saturation” regime, wherein increase in current do not result in any increase in contact voltage. Within the voltage saturation regime the coefficient of friction tends to be lower, a result that is attributed to the higher temperatures associated with the higher voltage (and resulting material softening). Higher interfacial temperatures also appear to be responsible for the higher wear rates observed at higher current levels as well as lower coefficients of friction for smoother surfaces in the presence of current.