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Certain coating applications including those used in aerospace, industrial maintenance, construction and transportation industries require a combination of primer/topcoat or basecoat/clear coat layers. These multilayered systems require a complex application and curing procedures. Multiple formulation, application and processing steps not only contribute to environmental waste generation and pollution they also use excessive amount of energy until a solid film has been produced. In addition, in most cases, including aerospace and industrial maintenance applications, the primer or undercoat must be topcoated within a specified period otherwise inter-coat adhesion will be compromised. It would be desirable to reduce the number of layers to a minimum while providing the same or better overall performance that current systems provide. In this paper we report the design and development of thermosetting polyurethane coatings that self-stratify to two distinct phases upon application and cure. Prototype pigmented systems were applied and cured and were characterized by FTIR, SEM/EDX and were evaluated using standard coating test methods.