The rapid development of the Internet of Things increases the demand for wearable devices. Compared with traditional chemical batteries, flexible thermoelectric technology contributes a solution for solving the power supply of wearable electronics. Here, we prepared n-type Bi2Te3 and p-type Bi0.5Sb1.5Te3 flexible thermoelectric films by the magnetron sputtering method, where the thermoelectric performance and their microstructures are systematically studied. The carrier concentration and mobility are optimized by adjusting the deposition temperature, eventually improving the thermoelectric performance and achieving the room-temperature power factors of 3.2 and 6.1 μW cm−1 K−2 for Bi2Te3 and Bi0.5Sb1.5Te3 films, respectively. Furthermore, after being bent 900 times with a radius of 5 mm, the resistance of these films barely increases, demonstrating the great potential for applications in wearable electronics. In order to further evaluate the practicability, these films are used to design a flexible thermoelectric generator, in which output performance improves with the increase in the temperature difference. The power density is up to ∼218.8 μW cm−2 at temperature differences of ∼41 K.
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