p-Type pseudo-binary alloys (Al 2 Te 3 ) x –(Bi 0.5 Sb 1.5 Te 3 ) 1−x (x=0∼0.2) were prepared by spark plasma sintering (SPS) technique and their thermoelectric properties were evaluated. Measurements show that the Seebeck coefficient decreases and electrical conductivity increases with Al 2 Te 3 content increasing due to a possible increment of free carrier (holes) concentration and establishment of special conducting mechanism upon adding Al 2 Te 3 . Thermal conductivity (κ) increases with temperature but reduces noticeably over the broad temperature range, such a reduction is directly attributed to the enhancement of phonon scattering resulted from both the precipitation of the second phase AlSb and nearly 12% atomic occupation of element Al in Te1 and Te2 sites in the crystal. The maximum ZT value of 0.86 can be obtained for x=0.1 at 419K, which is 0.28 higher than that of Bi 0.5 Sb 1.5 Te 3 under the same fabrication technology.