Engineering materials and devices can be damaged during their service life as a result of mechanical fatigue, punctures, electrical breakdown, and electrochemical corrosion. This damage can lead to unexpected failure during operation, which requires regular inspection, repair, and replacement of the products, resulting in additional energy consumption and cost. During operation in challenging, extreme, or harsh environments, such as those encountered in high or low temperature, nuclear, offshore, space, and deep mining environments, the robustness and stability of materials and devices are extremely important. Over recent decades, significant effort has been invested into improving the robustness and stability of materials through either structural design, the introduction of new chemistry, or improved manufacturing processes. Inspired by natural systems, the creation of self-healing materials has the potential to overcome these challenges and provide a route to achieve dynamic repair during service. Current research on self-healing polymers remains in its infancy, and self-healing behavior under harsh and extreme conditions is a particularly untapped area of research. Here, the self-healing mechanisms and performance of materials under a variety of harsh environments are discussed. An overview of polymer-based devices developed for a range of challenging environments is provided, along with areas for future research.