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   The Ag and In co‐doped PbTe, Ag_nPb₁₀₀In_nTe_100+2n(LIST), exhibitsn‐type behavior and features unique inherent electronic levels that induce self‐tuning carrier density. Results show that In is amphoteric in the LIST, forming both In³⁺and In¹⁺centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 10¹⁸cm⁻³at 323 K to ≈2.4 × 10¹⁹cm⁻³at 820 K, leading to large power factors peaking at ≈16.0 µWcm⁻¹K⁻²at 873 K. The lone pair of electrons from In⁺can be thermally continuously promoted into the conduction band forming In³⁺, consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm⁻¹K⁻¹. The addition of Ag creates spindle‐shaped Ag₂Te nanoprecipitates and atomic‐scale interstitials that scatter a broader set of phonons. As a result, a maximumZTvalue ≈1.5 at 873 K is achieved in Ag₆Pb₁₀₀InTe₁₀₂(LIST).

    

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