Zone-melted bismuth antimony telluride alloys have been the most widely applied commercial thermoelectric (TE) materials for decades. In this work it is demonstrated that hot deformation can enhance both TE properties and mechanical properties of zone-melted (Bi,Sb)2Te3 alloys. The hot deformation modifies the microstructure and induces a donor-like effect to adjust the carrier concentration and significantly reduce the lattice thermal conductivity. A high dimensionless figure of merit (ZT) of 1.36 at 400 K is obtained in Bi0.4Sb1.6Te3 after hot deformation, and also the average ZT is ∼1.2 in the temperature range of 300–525 K, which makes the alloy suitable for low temperature power generation.