The effects of copper oxide (CuO) on the microstructure and electric properties of nonstoichiometric compound terbium dioxide (Tb 4 O 7 ) ceramics were investigated. Results included a reduction in the sintering temperature to 1,100°C, a grain size of 4.2 lm, and a density of 96.2 %, which are larger than the values in previous investigation for Tb 4 O 7 ceramics (grain sizes between 0.4 and 1.0 lm). Among the sintered ceramics, the sample doped with 10.0 wt% CuO showed the maximum nonlinear coefficient a = 43.5, which is obviously greater than a = 3.03 of the pure sample. Doping with 10.0 wt% CuO also exhibited nonlinearity a = 2.14 even at 1,123 K. In addition, the impedance spectra of the sample doped with 5.0 mol% CuO showed the largest grain boundary semicircle; 0 and 20 % samples showed both inductive and capacitive reactance.