The inherently small temperature difference in air environment restricts the applications of thermoelectric generation in the field of Internet of Things and wearable electronics. Here, a leaf‐inspired flexible thermoelectric generator (leaf‐TEG) that makes maximum use of temperature difference by vertically aligning poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate and constantan thin films is demonstrated. Analytical formulae of the performance scales, i.e., temperature difference utilization ratio (φth) and maximum output power (Pmax), are derived to optimize the leaf‐TEG dimensions. In an air duct (substrate: 36 °C, air: 6 °C, air flowing: 1 m s−1), the 10‐leaf‐TEG shows a φth of 73% and Pmax of 0.38 µW per leaf. A proof‐of‐concept wearable 100‐leaf‐TEG (60 cm2) generates 11 µW on an arm at room temperature. Furthermore, the leaf‐TEG is flexible and durable that is confirmed by bending and brushing over 1000 times. The proposed leaf‐TEG is very appropriate for air convection scenarios with limited temperature differences.

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Realizing high‐temperature thermal stability in thermoelectric (TE) generators is a critical challenge. In this study, a synergistic interface and surface optimization strategy is implemented to enhance Mg3Sb1.5Bi0.5 TE generator performance by employing FeCrTiMnMg thermoelectric interface materials and the MgMn‐based alloy protective coating. The competitive output power density (ω) of 1.7 W cm−2 and a conversion efficiency (η) of 13% for the single‐leg device are achieved at hot‐side temperature (Th) and cold‐side temperature (Tc) of 500 and 5 °C, respectively. An ω of 0.8 W cm−2 and η of 6% for the two‐couple TE devices with p‐type commercial Bi2Te3 are also realized, values that are competitive with the commercial Bi2Te3 device. Additionally, the single‐leg device shows a high stable η for over 100 h when the Th and Tc are 400 and 5 °C, respectively, with an change rate (Δηmax/ηmax,o) of <3%. In situ transmission electron microscopy analysis further reveals that the high stability results from the effectively sluggish interdiffusion and reduced Mg evaporation that decrease the chemical potential gradient, reduce the saturated vapor pressure, and increase the diffusion activation energy barrier. This study provides a general technique route for boosting the high‐temperature thermal stability of TE generator.

The thermoelectric efficiency formula (η_max), derived by Ioffe, provides a direct connection between the material dimensionless figure of merit ZT and the maximum efficiency from heat into electricity in an...