A new inorganic binder system has been developed to prepare the mold having a high strength for the thin-walled casting. To increase the fracture strength at high temperature, a large amount of inorganic binder should be converted into glass phase and the generated glass phase has to be homogeneously coated on the surface of starting particles. In this work, two types of process were employed to investigate the coating and glassification efficiencies of inorganic precursor. In the first process (process I), the green body consisting of starting powder and organic binder was dipped in the inorganic precursor solution. In the second process (process II), the starting powder was coated by inorganic precursor, and then the organic binder was used to form the green body. The mold sample prepared using process II showed the higher strength value than that using process I, owing to the inclement effect on the glassfication efficiency by the loss of inorganic precursor in process I. The prepared real mold was perfectly produced and the casted product showed a clean surface without defects such as dross, nonmetallic inclusions, and crack. Consequently, the new inorganic binder system could be applied for preparing the mold for the thin-wall casting having high mechanical properties.