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A facile preparation method for flexible p-type CuI/polyvinylpyrrolidone (PVP) nanocomposite thermoelectric (TE) film is developed. First, CuI powder was synthesized by a one-pot method; second, PVP was coated in situ with the CuI powder; third, the CuI/PVP nanocomposite film was prepared on a nylon membrane by vacuum filtration and then hot-pressing. Transmission electron microscopy (TEM) observation indicates that the film consists of CuI nanograins with an average size of ~15 nm and PVP distributed at the inner wall of nanopores and the surface of the CuI nanograins. The composite film shows a large Seebeck coefficient of ~605 µVK⁻¹ and a power factor of ~8.05 µWm⁻¹K⁻² at 300 K. The nanocomposite film also exhibits excellent flexibility (~96% of initial electrical conductivity retention after being bent 1000 times along a 4 mm radius rod). A single-leg TE module outputs a voltage of ~3.6 mV when the temperature difference is 6 K. This work provides a fast, simple, and environmentally friendly method by which to prepare flexible CuI/PVP nanocomposite TE film with a large Seebeck coefficient, which could be used as a wearable sensor.