Starting from elemental powder mixture, ternary chromium chalcogenide CuCrSe2 has been synthesized facilely via the route of mechanical alloying and subsequent annealing. Effect of indium doping on the thermoelectric performance of CuCrSe2 has been studied detailedly. With the increase in indium doping content, the electrical resistivity decreases firstly until 0.25 at.% due to the electronegativity difference between In and Cr, and then increases due to the dissolution of indium and subsequent supersaturation precipitation of CuInSe2, and the Seebeck coefficient shows a similar trend with the electrical resistivity. The thermal conductivity increases firstly and then decreases with the increase in indium doping content due to the increasing phonon scattering by the CuInSe2 and CuCr(2)Se4. As a result, a maximum ZT of 0.65 at 673 K was achieved in the sample with 1.0 at.% In doping, which is enhanced almost 54% in compared with the In-free sample.