The influence of substrate type in boosting thermoelectric properties of co-evaporated Bi2Te3 and Sb2Te3 films (with 400 nm-thick) is here reported. Optimized power factor values are 2.7 × 10−3 W K−2 m−1 and 1.4 × 10−3 W K−2 m−1 for flexible Bi2Te3 and Sb2Te3 films, respectively. This is an important result as it is at least 2 times higher than the power factor found in the literature for flexible Bi2Te3 and Sb2Te3 films. A flexible infrared thermopile sensor was developed with high detectivity (2.50 × 107 cm √HzW−1).