Resistance to surface crystallization of polymer building coatings is a significant performance index for coating design. However, the high time expense of conventional surface crystallization experiments limits the efficiency of coating evaluation. In this study, an integrated experimental and modeling approach is proposed to evaluate surface crystallization on polymer coatings. Two models are developed as well as the surrogate-based optimization method is adopted to identify model parameters, and a transport-crystallization coupled model is constructed to predict the surface crystallization using the identified parameters. The effectiveness of the integrated approach is validated in three different coatings. It shows that the parameter identification method can estimate model parameters properly and provide good fitting results. In addition, the coupled model shows satisfactory accuracy when predicting surface crystallization. Furthermore, the analysis of the simulation results indicates that the coupled model could be instructive for coating design since it reveals the quantitative relationship between the surface crystallization resistance and macroscopic coating properties.