AbstractUse of a flexible thermoelectric source is a feasible approach to realizing self‐powered wearable electronics and the Internet of Things. Inorganic thin films are promising candidates for fabricating flexible power supply, but obtaining high‐thermoelectric‐performance thin films remains a big challenge. In the present work, a p‐type BixSb2−xTe3 thin film is designed with a high figure of merit of 1.11 at 393 K and exceptional flexibility (less than 5% increase in resistance after 1000 cycles of bending at a radius of ∼5 mm). The favorable comprehensive performance of the BixSb2−xTe3 flexible thin film is due to its excellent crystallinity, optimized carrier concentration, and low elastic modulus, which have been verified by experiments and theoretical calculations. Further, a flexible device is fabricated using the prepared p‐type BixSb2−xTe3 and n‐type Ag2Se thin films. Consequently, an outstanding power density of ∼1028 μW cm−2 is achieved at a temperature difference of 25 K. This work extends a novel concept to the fabrication of high‐performance flexible thin films and devices for wearable energy harvesting.
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