Dense 8 mol% CuO-doped 3Y-TZP ceramics were prepared by pressureless sintering for 8 h at 1500° and 1550°C, respectively. Transmission electron spectroscopy revealed that the ceramic sintered at 1500°C exhibits grain boundaries free of any amorphous phase, while crystalline copper-oxide grains were found in the zirconia matrix, whereas the sample sintered at 1550°C contains a Cu-rich amorphous grain boundary layer. The tribological behavior of these materials was tested under dry-sliding conditions using a pin-on-disk tribometer. The material sintered at 1500°C showed self-lubrication resulting in a low coefficient of friction (f) of 0.2–0.3 and a low specific wear rate (k) 10−6 mm3·(N·m)−1. In contrast, the material sintered at 1550°C showed poor tribological behavior (f=0.8–0.9; k 10−6 mm3·(N·m)−1 under the same conditions. The difference in the tribological behavior of these two materials was interpreted on the basis of mechanical properties and microstructural characteristics.