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Thermoelectric materials could play a crucial role in the future of wearable electronic devices. They can continuously generate electricity from body heat. For efficient operation in wearable systems, in addition to a high thermoelectric figure of merit, zT, the thermoelectric material must have low thermal conductivity and a high Seebeck coefficient. In this study, we successfully synthesized high-performance nanocomposites of n-type Bi2Te2.7Se0.3, optimized especially for body heat harvesting and power generation applications. Different techniques such as dopant optimization, glass inclusion, microwave radiation in a single mode microwave cavity, and sintering conditions were used to optimize the temperature-dependent thermoelectric properties of Bi2Te2.7Se0.3. The effects of these techniques were studied and compared with each other. A room temperature thermal conductivity as low as 0.65 W/mK and high Seebeck coefficient of −297 μV/K were obtained for a wearable application, while maintaining a high thermoelectric figure of merit, zT, of 0.87 and an average zT of 0.82 over the entire temperature range of 25 °C to 225 °C, which makes the material appropriate for a variety of power generation applications.