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We synthesized the solid solutions CuGa1-xInxTe2 (x = 0-1.0) by isoelectronic substitution of element In (Ga) for Ga(In) in the CuMTe2 (M = Ga, In) lattices and examined their thermoelectric properties. The structure upon substitution provides much high Seebeck coefficient (α), relatively low thermal (κ), and electrical conductivity (σ). AT 701 K, the α, σ, and κ are 283.15 µV K-1, 1.15 × 104 Ω-1 m-1, and 0.71 W m-1 K-1, respectively, for CuGa0.36In0.64Te2, which give the figure of merit (ZT) of 0.91, about two times those of the mother compounds CuGaTe2 and CuInTe2. This material holds great application perspectives at intermediate temperatures. [ABSTRACT FROM AUTHOR]