CuCrSe2compounds were synthesized by mechanical alloying followed by annealing and spark plasma sintering at temperatures of 873 K, 923 K, 973 K and 1023 K. Our investigation revealed that high SPS temperature (above 973 K) is the key to obtaining CuCrSe2single phase completely free of a metallic secondary phase CuCr2Se4. The ultralow thermal conductivity caused by the Cu ions disorder, complex layered structure and dislocation leads to the favorable thermoelectric performance in CuCrSe2compound. A maximum ZT value over 0.75@873 K is achieved in the absolutely pure sample sintered at 1023 K. © 2016 Acta Materialia Inc.