"Self-healing metals" - Modern materials contain extraordinary levels of complexity with components spanning a hierarchy of length scales. Designing materials that contain complex microstructures and demonstrate unique behaviors would be difficult solely using a reductionist approach to materials development. Although this approach has led to many technological breakthroughs, the rapid evolution of technology and the need for a shortened materials development cycle are driving materials scientists toward a more predictive approach based on design. Our research lies in the basic understanding of the relationship between processing, structure, properties and performance. We use a systems-based materials design approach that couples experimental research with theory and mechanistic modeling for the accelerated development of materials. Microstructural properties are modeled using a toolbox of design models and methods that are strongly tied to materials science. These properties can then be expressed as thermodynamic parameters that can be predicted by using computational thermodynamic tools. Prototypes are then created to experimentally analyze and validate the design models that feed back into the working design for optimizing materials performance while minimizing design iterations. With a clear guide for materials design, large-scale experiments can be avoided while promoting the rapid development of complex materials. This talk focuses on the development of two smart technologies, high strength shape memory alloys and self-healing metal matrix composites (MMC). The topic of high performance shape memory alloys centers on the development of a NiTiHfZr alloy for high strength and temperature actuators. Meanwhile, self-healing alloys have the potential to demonstrate extraordinary properties including, but not limited to, healing, high strength and toughness. This talk seeks to present the challenges and opportunities in the design of both systems as well as, shed new light on the potential of a thermodynamically driven design approach in developing materials with unique behaviors.