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Self-powered wearable electronics require thermoelectric materials simultaneously with a high dimensionless figure of merit ( zT ) and good flexibility to convert the heat discharged by the human body into electricity. Ag 2 (S,Se)-based semiconducting materials can well satisfy these requirements, and thus, they are attracting great attention in thermoelectric society recently. Ag 2 (S,Se) crystalizes in an orthorhombic structure or monoclinic structure, depending on the detailed S/Se atomic ratio, but the relationship between its crystalline structure and mechanical/thermoelectric performance is still unclear to date. In this study, a series of Ag 2 Se 1‐ x  S  x   ( x  = 0, 0.1, 0.2, 0.3, 0.4, and 0.45) samples were prepared and their mechanical and thermoelectric performance dependence on the crystalline structure was systematically investigated.  x  = 0.3 in the Ag 2 Se 1‐ x  S  x   system was found to be the transition boundary between orthorhombic and monoclinic structures. Mechanical property measurement shows that the orthorhombic Ag 2 Se 1‐ x  S  x   samples are brittle while the monoclinic Ag 2 Se 1‐ x  S  x   samples are ductile and flexible. In addition, the orthorhombic Ag 2 Se 1‐ x  S  x   samples show better electrical transport performance and higher  zT  than the monoclinic samples under a comparable carrier concentration, most likely due to their weaker electron-phonon interactions. This study sheds light on the further development of flexible inorganic TE materials.

Crystalline Structure-Dependent Mechanical and Thermoelectric Performance in Ag2Se1‐xSx System