The flexible thermoelectric (TE) cooling and energy harvesting devices made of p-and n-type TE materials have great potential for the applications in wearable and portable electronics, as they can directly realize mutual conversion between thermal energy and electrical energy without mechanical moving parts or toxic liquids; [1-4] Recently, flexible TE materials have evoked researchers' great interest, and many efforts have been made to improve their TE properties, which is estimated by the figure-of-merit value, ZT ¼ S 2 σT/κ (κ, T, σ, and S are the thermal conductivity, absolute temperature, electrical conductivity, and Seebeck coefficient, respectively). [2,4] Conducting polymers have good flexibility and process ability, which are suitable for preparation of flexible TE materials; [5,6] however, the TE properties of conducting polymers are still much lower when compared with traditional inorganic TE materials. [5] It is an effective approach to improve the conducting polymers' TE performance by preparation of inorganic/conducting polymer composites via a suitable process. [1,7] The most frequently used methods for preparation of inorganic/polymer composites are consisting of the solution mixing, [8] mechanical blending, [9] spin-coating, [10] drop-casting, [11] in situ polymerization, [12] gas-phase polymerization, [13] vacuum filtration, [14] 3D printing, [15] etc. As one of the most promising conducting polymers, poly(3, 4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS), has many advantages, e.g., water solubility, commercial availability, mechanical flexibility, and low intrinsic thermal conductivity. [14,16,17] PEDOT:PSS has, therefore, been commonly used as matrixes for preparation of inorganic/conducting polymer composites. [5] The morphologies of inorganic fillers, such as nanoparticles (NPs), nanosheets (NSs), nanowires (NWs), have significantly affected their dispersibility in conducting polymer matrix and TE properties of the as-prepared composites. [14,18,19] BiTe based alloy NSs, Sn-Se based alloy NSs, and MoS 2 NSs, etc., after exfoliation for their corresponding particles, can be dispersed in a suitable solvent, e.g., ethanol, N-methyl-2-pyrrolidone, or N, N-dimethylformamide.