BiTe-based alloys have historically dominated the commercial sector of near-ambient-temperature thermoelectric technology. However, the massive intrinsic defects form the "donor-like" effect and affect the transport properties of BiSbTe significantly. Here, it is demonstrated that the over-stoichiometric Sb fills Te vacancies and weakens the defect scattering, resulting in a desirable carrier mobility. The boost-generated antisite defects also compensate for the extra hole carries. Combined with dilute Cu doping, the global microstructural modulation is synergistically promoted, characterized by Sb coherent nanoprecipitates and high-density twins. Benefitting from the decoupled electrical-thermal transport, the peak ZT is improved to ≈1.50 at 350 K, with an average ZT of 1.25 from 300 to 500 K. The further designed and integrated 17-pair power generators exhibit ultrahigh conversion efficiency, reaching 6.7% under a 200 K temperature gradient, and show excellent operational stability. These achievements hold great potential for advancing BiTe-based power generators in low-grade waste heat recovery.
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