Current thermoelectric (TE) materials often have low performance or contain less abundant and/or toxic elements, thus limiting their large-scale applications. Therefore, new TE materials with high efficiency and low cost are strongly desirable. Here we demonstrate that, SiS and SiSe monolayers made from non-toxic and earth-abundant elements intrinsically have low thermal conductivities arising from their low-frequency optical phonon branches with large overlaps with acoustic phonon modes, which is similar to the state-of-the-art experimentally demonstrated material SnSe with a layered structure. Together with high thermal power factors due to their two-dimensional nature, they show promising TE performances with large figure of merit (ZT) values exceeding 1 or 2 over a wide range of temperatures. We establish some basic understanding of identifying layered materials with low thermal conductivities, which can guide and stimulate the search and study of other layered materials for TE applications.2 Thermoelectric materials have great potential for novel energy and environmental applications and have been extensively studied recently. The performance of a TE material is usually evaluated by the dimensionless figure of merit, which is denoted as ZT and defined as ZT = (S / ) , where S, σ, κ and T are the Seebeck coefficient, the electrical conductivity, the thermal conductivity (including both electronic contribution and lattice contribution ), and the average working temperature, respectively. [1][2][3][4] The product S σ is also known as the power factor (PF). To be an ideal TE material with high heat-to-electric conversion efficiency, a high ZT value, i.e., larger than unity, is required.Currently, two strategies are usually considered to enhance ZT of a TE material. One is to enhance the Seebeck coefficient or the PF using band structure engineering methods, [5] such as modifying the electronic density of states and Fermi energy through doping heteroatoms, reducing crystal symmetry to achieve high band edge degeneracy, [6][7][8] etc. The other is to reduce thermal conductivity using methods such as nanostructuring, [9][10][11][12][13][14][15][16][17][18][19][20][21] alloying, [14,[22][23][24][25][26] etc. These strategies have achieved significant progress in the past decade. However, most of now-existing TE materials, including PbTe, Bi 2 Te 3 and complex structure based TE materials, [3] strongly rely on heavy elements and/or rare-earth metals, which often have low abundance or are toxic, [3] thus limiting the large-scale employment of TE materials. Consequently, it will be of great importance to explore new TE materials not only with a high maximum ZT over a wide range of temperatures, but also made from non-toxic and earth-abundant elements.Recently, those materials with layered structures have shown such promise. As an experimentally demonstrated state-of-the-art thermoelectric material, SnSe has a simple layered structure similar to black phosphorus and only contains earth-abundant and non-toxic ...