Vertical Bridgman systems with programmable temperature control are used to grow (SbxBi1:x)2Te3crystals. High purity Bi, Sb and Te are used as sources and the diameter of 1.1 cm, little soft bulk crystals of (SbxBi1–x)2Te3can be obtained. Scanning electron microscope (SEM) and electron probe microanalysis (EPMA) are used to analyze the micro‐structure and the compositions of the crystal. From the X‐ray diffraction patterns it appears that the grown crystal is single crystal or directive polycrystal. If the uniformity of the source solution and grown temperature are under control, then the high quality of single crystals can be obtained. The dependence of crystal structure and the thermoelectric characteristics on the changed compositions of grown crystals are discussed. The optimum composition for the thermoelectric properties is Sb1.00Bi1.04Te2.96. When the DC current, 3A, is applied to the Sb1.00Bi1.04Te2.96crystal with suitable electrodes, the temperature difference (△T) between two sides of the crystal can be as high as 60°C. It is 2 times larger than that ever obtained by Sb2Te3crystal. It appeared that the grown (SbxBi1‐x)2Te3crystals have the potential on the fabrication of thermoelectric devices and electronic cooling system.