A significant enhancement in the thermoelectric performance was observed for three-dimensional conducting aerogels, which were obtained from poly(3,4-ethylenedioxythiophene) : poly(4-styrenesulfonic) (PEDOT:PSS) and multiwalled carbon nanotubes (MWCNTs) suspensions by adding different concentrations of metallic silver (Ag). It was found that the electrical conductivity and Seebeck coefficient could be simultaneously increased with the unique structure. Moreover, the conducting aerogels have an ultralow thermal conductivity (0.06 W m −1 K −1 ) and a large Brunauer-Emmett-Teller surface area (228 m 2 g −1 ). The highest figure of merit (zT) value in this study was 7.56×10 −3 at room temperature upon the addition of 33.32 wt.% Ag. Although the zT value was too low, our work may provide new insights into the design and development of the thermoelectric material for applications. Further investigation with PEDOT:PSS aerogels will be continued to get an economical, lightweight, and efficient polymer thermoelectric material.