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Polycrystalline-sintered samples of thallium based substances, (Tl2Te)100−x(Sb2Te3)x (x= 0, 1, 5, 10), were prepared by melting Tl2Te and Sb2Te3 ingots followed by annealing in sealed quartz ampoules. The thermoelectric properties were measured from room temperature to around 600 K. The values of the Seebeck coefficient of all samples are positive, indicating a p-type conduction characteristic. The maximum value of the power factor is 6.53×10−4 Wm−1K−2 at 591 K obtained for x= 10 (Tl9SbTe6), which is about one order lower than those of state-of-the-art thermoelectric materials. All samples indicate an extremely low thermal conductivity, for example that of Tl2Te is approximately 0.35 Wm−1K−1 from room temperature to around 600 K. Although the electrical performance of the samples is not so good, the ZT value is relatively high due to the extremely low thermal conductivity. The maximum ZT value is 0.42 at 591 K obtained for Tl9SbTe6.