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P-type Sb 2 Te 3 has been recognized as a potential thermoelectric material for applications in low-medium temperature ranges. However, its inherent high carrier concentration and lattice thermal conductivity led to a relatively low ZT value, particularly around room temperature. This study addresses these limitations by leveraging high-energy ball milling and rapid hot-pressing techniques to substantially enhance the Seebeck coefficient and power factor of Sb 2 Te 3 , yielding a remarkable ZT value of 0.55 at 323 K due to the donor-like effect. Furthermore, the incorporation of Nb─Ag co-doping increases hole concentration, effectively suppressing intrinsic excitations ≈548 K while maintaining the favorable power factor. Simultaneously, the lattice thermal conductivity can be significantly reduced upon doping. As a result, the ZT values of Sb 2 Te 3 -based materials attain an impressive range of 0.5-0.6 at 323 K, representing an almost 100% improvement compared to previous research endeavors. Finally, the ZT value of Sb 1.97 Nb 0.03 Ag 0.005 Te 3 escalates to 0.92 at 548 K with a record average ZT value (ZT avg ) of 0.75 within the temperature range of 323-573 K. These achievements hold promising implications for advancing the viability of V-VI commercialized materials for low-medium temperature application., (© 2023 Wiley‐VCH GmbH.)