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Thermoelectric materials, capable of interconverting heat and electricity, are attractive for applications in thermal energy harvesting as a means to power wireless sensors, wearable devices, and portable electronics. However, traditional inorganic thermoelectric materials pose significant challenges due to high cost, toxicity, scarcity, and brittleness, particularly when it comes to applications requiring flexibility. Here, we investigate organic–inorganic nanocomposites that have been developed from bespoke inks which are printed via an aerosol jet printing method onto flexible substrates. For this purpose, a novel in situ aerosol mixing method has been developed to ensure uniform distribution of Bi2Te3/Sb2Te3 nanocrystals, fabricated by a scalable solvothermal synthesis method, within a poly(3,4-ethylenedioxythiophene) polystyrene sulfonate matrix. The thermoelectric properties of the resulting printed nanocomposite structures have been evaluated as a function of composition, and the power factor was found to be maximum (∼30 μW/mK2) for a nominal loading fraction of 85 wt % Sb2Te3 nanoflakes. Importantly, the printed nanocomposites were found to be stable and robust upon repeated flexing to curvatures up to 300 m–1, making these hybrid materials particularly suitable for flexible thermoelectric applications.