Nowadays, it is still a challenge to prepare flexible sensors with great mechanical strength, stretchability, high sensitivities, and excellent self-healing (SH) abilities. Herein, a nanostructured supramolecular elastomer is reported with a dual noncovalent network of hydrogen bonding interactions and metal-ligand coordination. The resultant flexible sensor presents ultrafast (30 s), autonomous, and repeatable SH ability with high healing efficiency (80% after the 3rd healing process), as well as enhanced mechanical properties. Benefitting from the 3D conductive network, the sensor exhibits high electrical sensitivity and very low detection limit (0.2% strain). As a result, the flexible sensor is capable of precisely monitoring small strains of human motions (such as vocal-cord vibration), and exhibits reproducible and recognizable current signals after cutting-healing process. The dual noncovalent network design proposed here opens up a new opportunity for scalable fabrication of high performance SH sensors and other electronic devices.