LAUSR

To realize thermoelectric textiles that can convert body heat to electricity, fibers with excellent mechanical and thermoelectric properties are needed. Although poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is among the most promising organic thermoelectric materials, reports that explore its use for thermoelectric fibers are all but absent. Herein, the mechanical and thermoelectric properties of wet‐spun PEDOT:PSS fibers are reported, and their use in energy‐harvesting textiles is discussed. Wet‐spinning into sulfuric acid results in water‐stable semicrystalline fibers with a Young's modulus of up to 1.9 GPa, an electrical conductivity of 830 S cm−1, and a thermoelectric power factor of 30 μV m−1 K−2. Stretching beyond the yield point as well as repeated tensile deformation and bending leave the electrical properties of these fibers almost unaffected. The mechanical robustness/durability and excellent underwater stability of semicrystalline PEDOT:PSS fibers, combined with a promising thermoelectric performance, opens up their use in practical energy‐harvesting textiles, as illustrated by an embroidered thermoelectric fabric module.