Organic thermoelectric devices (OTEDs) are recognized one of the next generation energy conversion platforms because of their huge potentials for securing electricity continuously from even tiny heat sources in our daily life. The advantage of OTEDs can be attributable to the design freedom in device shapes and the low-cost fabrication by employing solution coating processes at low temperatures. As one of the major OTE materials to date, poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has been used, but no study has been yet carried out on its acidity control even though the acidic components in OTEDs can seriously affect the device performance upon operation. Here we demonstrate that the addition of aniline (a weak base) can control the acidity of PEDOT:PSS and enhance the performance of OTEDs. In particular, the vertical OTEDs with aniline-doped PEDOT:PSS films (active area = 1.0 cm2) could continuously generate electricity (0.06 nW) even at low temperatures (<38 °C) when they were mounted on a desk lamp (power = 24 W).