 Abstract advanced elastomers are increasingly used in emerging areas, for example, flexible electronics and devices, and these real-world applications often require elastomers to be stretchable, tough and fire safe. To date, however, there have been few successes in achieving this performance portfolio due to differing governing mechanisms. This paper reports on a new type of stretchable, super-tough, and self-extinguishing polyurethane elastomer with dynamic pi-pi stacking motifs and phosphorus-containing moieties. The resultant elastomer has a large break-strain of approximately 2,260%, a record-high toughness of around 460 mj-slash-m superscript 3, and a self-extinguishing capability due to the presence of both phosphorus-containing units and pi-pi stacking interactions. These properties make it suitable for use in flexible electronics and devices. This article was authored by Jiaoshui, Zhenyu Lin, Tao Wan, and others.