Abstract: Using the data of rare-earth containing phosphors, VPTC materials and cathode materials of Ni/H batteries as examples, the modeling methods of linear PLS method, PLS method with non-linear terms, and non-linear PLS-ANN method are investigated by comparison of their effectiveness in optimization of material design. Results show that when non-linear relationship between the material properties and the influential factors is obvious, non-linear PLS-ANN method is more suitable for model building. Their calculated values are in agreement with the experimental values.