Carbon Nanotube–Polyurethane Composite Sheets for Flexible Thermoelectric Materials

[Image: see text] Integration of single-wall carbon nanotubes (SWCNTs) in the form of fabriclike sheets or other preformed assemblies (films, fibers, etc.) simplifies their handling and allows for composites with higher nanotube contents, which is needed to better exploit their outstanding properties and achieve multifunctional materials with improved performance. Here, we show the development of p-type SWCNT–thermoplastic polyurethane (TPU) fabric materials with a wide range of SWCNT contents (from 5 to 90 wt %) by employing a one-step filtration method using a suspension of SWCNTs in a TPU solvent/nonsolvent mixture. The mechanical and thermoelectric (TE) properties of these SWCNT–TPU nanocomposites were tailored by varying the SWCNT/TPU wt % ratio, achieving significant advantages relative to the pristine SWCNT buckypaper (BP) sheets in terms of strength and stretchability. In particular, the SWCNT–TPU nanocomposite with a 50/50 wt % ratio composition (equivalent to 15 vol % of SWCNTs) shows a power factor (PF) of 57 μW m(–1) K(–2), slightly higher compared to the PF of the SWCNT BP prepared under the same conditions (54 μW m(–1) K(–2)), while its mechanical properties significantly increased (e.g., ∼7-, 25-, and 250-fold improvements in stiffness, strength, and tensile toughness, respectively). These results represent a significant step toward the development of easy-to-process self-supporting and stretchable materials with robust mechanical properties for flexible thermoelectric devices.