Using special testers, the triboelectric behaviors of several materials were investigated in this paper under the conditions of high speeds and large currents. The obtained results revealed that the tribological behaviors and current-conducting characteristics have complicated interrelationships. Worsening in the servicing conditions can obviously deteriorate the tribological as well as electrical behaviors; high sliding speeds and large electrical currents can worsen the tribological and electrical conductivity properties, while an appropriate contact pressure can benefit the electrical contact properties. Further analyses reveal that the worsening effects of the above factors, such as frictional heat, arc discharge, arc heat, and surface morphology, result in poor triboelectric contact performance. Among these, the electric arc is one of the most serious factors, because the occurrence of an electric arc may cause severe oxidation, melting, and roughening of the contact surface, thereby causing deterioration in the current-conducting quality as well as material loss.