adversely function as coolers, belong to an important category of advanced energy materials for sustainable energy utilization. [2] The performance of TE materials is generally assessed by the dimensionless figure of merit:where S, σ, T, and κ are the Seebeck coefficient, electrical conductivity, absolute temperature, and thermal conductivity, respectively. [3] The ideal TE materials are suggested to behave as "electronic crystal and phonon glass." [4] Compared to the traditional inorganic TE materials such as Bi 2 Te 3 or PbTe, which are still the most used commercial materials with the state-of-art ZT values, conducting polymer based TE materials are more like "phonon glass" with intrinsic low thermal conductivity. They emerge as a quite promising new type of TE materials due to their unique advantages, such as abundant sources, light weight, solution processibility for mass production, flexibility, mechanical robustness, and so on.One important merit for the conducting polymer as good candidate of TE material is the easy modulation of the energy levels which shall result in wide range change of S and σ, enabling huge room to improve the power factor (PF, defined as S 2 σ). Recent breakthrough in conducting polymer poly(3,4-ethylenedioxythiophene) through a control of the oxidation level and high-boiling-point solvents treatment reported a record high ZT value of 0.42 at room temperature. [5] Another parallelly developed strategy is to incorporate nanostructured inorganics with high electrical conductivity or high Seebeck coefficient in conducting polymer to form hybrid nanomaterials, where the presence of rich interfacial interfaces offer new opportunities to decouple the TE property parameters, showing great promise for high-performance TE conversion. So far, the successful choice of inclusions for high-performance polymer-based TE hybrid materials has been limited to Te, Bi 2 Te 3 , and carbon nanotube (CNT)/graphene. [6] Among these hybrid materials, Te/polymer hybrids show promising ZT values (≈0.1-0.2); however, the problem is that high Te content (as high as 70-90 wt%) is needed to achieve high thermopower and PF value (i.e., >100 µW m −1 K −2 ). [3,[7][8][9] Since the natural abundance of Te is as Recent developed conducting polymer based hybrid thermoelectric (TE) materials provide a promising alternative route for energy conversion on a large scale. However, high thermopower largely relies on high content of lowabundance elements, such as tellurium, which impedes the mass production of these materials. To optimize the compositions of the hybrids and further improve the TE properties, interfacial engineering is therefore employed to modulate the carrier transport properties in rationally designed multiwalled carbon nanotubes (MWCNTs)-Te nanorod/polyaniline (PANI) ternary hybrid nanomaterials considering the similar π-π conjugated interactions among these constituents. The effects of MWCNTs and Te nanorods, especially the multiple interfaces formed between the constituents, on the TE performances and ca...