Thermoelectric (TE) energy harvesting, which converts available thermal resources into electrical energy, is attracting significant attention, as it facilitates wireless and self-powered electronics. Recently, as demand for portable/wearable electronic devices and sensors increases, organic-inorganic TE films with polymeric matrix are being studied to realize flexible thermoelectric energy harvesters (f-TEHs). Here, we developed flexible organic-inorganic TE films with p-type Bi0.5Sb1.5Te3 powder and polymeric matrices such as poly(3,4-eethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) and poly (vinylidene fluoride) (PVDF). The fabricated TE films with a PEDOT:PSS matrix and 1 wt% of multi-walled carbon nanotube (MWCNT) exhibited a power factor value of 3.96 μW ‧ m-1 ‧ K-2 which is about 2.8 times higher than that of PVDF-based TE film. We also fabricated f-TEHs using both types of TE films and investigated the TE output performance. The f-TEH made of PEDOT:PSS-based TE films harvested the maximum load voltage of 3.4 mV, with a load current of 17.4 μA, and output power of 15.7 nW at a temperature difference of 25 K, whereas the f-TEH with PVDF-based TE films generated values of 0.6 mV, 3.3 μA, and 0.54 nW. This study will broaden the fields of the research on methods to improve TE efficiency and the development of flexible organic-inorganic TE films and f-TEH.