Process parameters of nanostructured ZrO2-7%Y2O3 coating during plasma spraying on the properties of the coating was optimized based on simulated annealing algorithm. BP neural network was applied to compute fitness of simulated annealing algorithm. A BP neural network model was built, four process parameters were input , the parameters included spraying distance, spraying electric current, primary gas pressure and secondary gas pressure, bonding strength of coating was output. Network was trained by orthogonal test data. Process parameters of coating were optimized by simulated annealing algorithm. The results show that maximal bonding strength of coating is 43.0377MPa. Process parameters for plasma spraying nanostructured ZrO2-7%Y2O3 coating are spraying distance of 80mm, spraying electric current of 977.0283A, primary gas pressure of 0.3046MPa and secondary gas pressure 0.9886MPa.