Current azeotropic refrigerant R410A has the disadvantage of a high GWP. Thus, a reliable predictive model is necessary to be developed for screening of the alternative refrigerant mixtures with low boiling point. In this work, a database of binary refrigerant azeotropic mixtures is identified by experiments and used to verify the feasibility of using COSMO-based models to predict the VLE of binary refrigerant mixtures. It contains 1766 compounds, out of which 306 are known as refrigerants. Sixty-nine binary systems are then selected after excluding the systems containing water and those with incomplete and azeotropic temperatures exceeding 325 K. The COSMO-based models were tested and found to predict the azeotropic points qualitatively for the binary refrigerant systems. Thus, all the VLE data of binary refrigerant systems in the database can be predicted through the combination of COSMO-SAC and COSMO-RS models. Next, three binary azeotropic refrigerant mixtures that could be a potential replacement for R410A were identified and their performance verified through simulation of the refrigeration process.