Coating slurry, in which the infrared radiation material is the main content, is applied in industrial furnaces to improve heat transfer and raise efficiency of furnaces. In this study, a Cu x Co 1 − x Fe 2 O 4 series material with a spinel structure was prepared, and the emissivity of different formulas in two wavebands (3–5 μm and 8–14 μm) was measured. To ensure that the material delivered high emissivity, optimization models were proposed using Matlab software, and proportions of CuO, Co2O3 and Fe2O3 were found to be 16.98%, 16.73% and 66.29%, respectively, in the optimal formula. Thus, using the Cu x Co 1 − x Fe 2 O 4 series material and additives, according to mixture regression method, fifteen formulas of coating slurry were designed, prepared and the emissivities were measured. With the Matlab software optimization model, the content of coating slurry was optimized and the corresponding emissivities were measured to be 0.931 and 0.905 in two wavebands, which is in agreement with the optimized calculation.