Green pigments have been synthesized. Sodium silicate, chromium oxide, lithium carbonate and quartz were used as the main raw materials to prepare (Na0.4Li0.6)CrSi2O6 emerald green pigments by solid state reaction under the non-reductive conditions. The effects of the various technological conditions, such as raw materials ratios of (Na0.4Li0.6)/Cr/Si, calcination temperature, holding time and the type of mineralizers, on the color presentation of the synthesized pigments were studied. XRD and SEM were employed to analyze the crystalline and structure of the synthesized pigments. Chroma value was used to characterize the color of the pigments. The results show that the optimized (Na0.4Li0.6)CrSi2O6 pigments with chroma value of L*=57.78, a*=-18.98~-18.68 and b* = 10.88~9.01 were obtained.