the Seebeck coefficient drops as shown in Figure 1a. [1,2] At the same time, the thermal conductivity from electrons (κ e ) will also increase according to the Wiedemann-Franz law. As a result of these interdependencies, good thermoelectric materials are typically narrow-bandgap semiconductors. This is because wide-bandgap semiconductors are relatively difficult to be highly doped, [3] hence limiting their ability to achieve optimized electrical conductivity for high powerfactor (S 2 σ). They are also typically composed of light elements, which translates to relatively high thermal conductivity. In the other extreme, metals or semi-metals have too large a carrier density or sometimes bipolar carriers, and their density of states (DOS) typically varies slowly at the Fermi level, which results in a low Seebeck coefficient. Additionally, to first order, the Seebeck coefficient typically peaks at S max ∼ E g /2eT max , where E g is the bandgap and T max is the temperature at which S max is located, although more accurate estimates can be made. [4] Therefore, narrow-bandgap semiconductors composed of heavy elements have been the focus in the search for high-performance thermoelectric materials, especially for low-to-intermediate temperature applications.However, layered materials could offer a new platform where relatively high electrical conductivity coexists with high Seebeck coefficient. One of the advantages for layered materials is the quantum size effect. [5] The fact that layered materials are atomically thin layers held together by weak vdW forces indicates that free carriers residing in each layer experience strong quantum confinement, akin to that in 2D. This is especially true for monolayers that can be isolated from the layered materials. As a result, the DOS of these 2D (or quasi-2D) systems significantly deviate from that of a 3D, bulk material, exhibiting strong anisotropy. For example, in the basal plane, sharp rises and peaks could develop in the DOS, different from the smooth DOS in 3D materials. Such rapidly varying DOS (with respect to electron energy E, i.e., high dDOS/dE) is beneficial for thermoelectricity. This is because when the Fermi level (E F ) is tuned to these positions in the DOS, a large asymmetry exists between hot (E > E F ) and cold (E < E F ) electrons, hence more effectively transporting entropy per charge, resulting in a higher Seebeck coefficient without a large sacrifice in the electrical conductivity. Meanwhile, the tunability of the Fermi level of the layered materials can be accessed much more easily than bulk materials by introducing intercalated ions or an electric field effect which assists in optimizing the Seebeck coefficient. [6][7][8][9][10] Another Layered materials have garnered immense interest due to their unique electronic, mechanical, thermal, and optoelectronic properties. In these materials, atomically thin layers are held together by van der Waals (vdW) interactions, allowing single layers to be isolated and studied as 2D materials. New theoretical insights a...