Fe addition up to x=0.1 in CuAl 1−x Fe x O 2 (0≤x≤0.2) led to an increase in electrical conductivity with an increase in Fe content because of increases in the grain size, density, and carrier density. On the other hand, Fe substitution up to x=0.1 caused a decrease in the Seebeck coefficient due mainly to an increase in carrier density. The highest value of power factor (1.1×10 −4 Wm −1 K −2 ) was attained for CuAl 0.9 Fe 0.1 O 2 at 1140K. We have demonstrated in the present study that Fe addition is highly effective for enhancing high-temperature thermoelectric properties of CuAlO 2 .