Electrical behaviors of plasma-sprayed Al₂O₃-TiO₂ coatings have been investigated in terms of their TiO₂ content. On increasing the TiO₂ content from 6 to 30 wt%, the DC electrical conductivity increased by several orders of magnitude. From impedance spectroscopy analysis, the total conductivity of the grains and grain boundaries and their respective activation energies were determined without the electrode effects that could impede ionic transfer. An electron transference number was also estimated, ranging between 6.5% and 7.3% for 13 wt% TiO₂ and between 0.4% and 0.7% for 30 wt% TiO₂ in the coating. Because of the high electronic contribution to the total conductivity, the Al₂O₃-TiO₂ coating could be a new candidate material to obtain superior electrical conductivity as well as corrosion and wear resistances.