Bismuth telluride alloys have dominated the industrial application of thermoelectric cooling, but the relatively poor mechanical performance of commercial zone-melting material seriously limits the device integration and stability. Here, we exhibit synergistically enhanced thermoelectric and mechanical performances of sintered Bi0.48Sb1.52Te3–AgSbSe2 composites. It is found that the increased hole concentration improves the S2σ to 40 μW cm–1 K–2 at room temperature, and the emerged various defects effectively suppress the κl to 0.57 W m–1 K–1 at 350 K. All effects harvest a highest ZT = 1.2 at 350 K along with an average ZT = 1.0 between 300–500 K in the x = 0.2 sample. Notably, AgSbSe2 addition not only optimizes the thermoelectric properties, but also enhances the mechanical performance with a Vickers hardness of 0.75 GPa. Furthermore, the isotropy of thermoelectric properties is also observably promoted by solid-phase reaction combined with high-energy ball milling and hot pressing. Our study reveals a viable strategy to improve the comprehensive performance of sintered bismuth telluride materials.