Thermoelectric inorganic films are flexible when sufficiently thin. By removing the substrate, that is, making them free-standing, the flexibility of thermoelectric films can be enhanced to the utmost extent. However, studies on the flexibility of free-standing thermoelectric inorganic films have not yet been reported. Herein, the high thermoelectric performance and flexibility of free-standing thermoelectric Ag2Se films are reported. Free-standing Ag2Se films with a thickness of 25.0 ± 3.9 μm exhibited an in-plane zT of 0.514 ± 0.060 at room temperature. These films exhibited superior flexibility compared to Ag2Se films constrained on a substrate. The flexibility of the Ag2Se films was systematically investigated in terms of bending strain, bending radius, thickness, and elastic modulus. Using free-standing Ag2Se films, a substrate-free, flexible thermoelectric generator was fabricated. The energy-harvesting capacity of the thermoelectric generator was also demonstrated.

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