A one-pot cascade strategy for the synthesis of 2-aminothiazole derivatives by tertiary enaminones, KSCN, and anilines was developed. By changing the reaction temperature, the three-component reaction could be transformed in different ways to obtain moderate to good yields of polysubstituted 2-aminothiazoles and 2-iminothiazolines. This protocol provides an efficient and concise approach to accessing 2-aminothiazole derivatives with potential bioactivity from readily accessible building blocks and reagents.