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α-In2Se3 is of large bandgap (∼1.4 eV) semiconductor and its structure is based on two-layer hexagonally packed arrays of selenium atoms with 1/3 of the sites of indium atoms being empty. Here we report a bandgap Eg reduction due mainly to the formation of a Cu2Se slab in the host In2Se3, which is responsible for the remarkable improvement of thermoelectric performance of bulk polycrystalline In2-xCuxSe3 (x = 0.1-0.2). When x = 0.2 the dimensionless figure of merit ZT and power factor were increased by a factor of 2 and 3, respectively, at 846 K if compared to those of Cu-free In2Se3. Interestingly, an incorporation of Cu into the lattice of In2Se3 results in a change in morphology from amorphouslike structure represented by In2Se3 to a visible polycrystalline form attributed to partial crystallization of the structure. This change enhances lattice thermal conductivities κL over the very low values of In2Se3. However, the enhancement is only moderate because of the effective scattering of phonons in the polycrystalline nanostructure. [ABSTRACT FROM AUTHOR]