Dynamic Self‐Healing Polymer Architectures for High‐Performance Flexible Sensing

Abstract

ABSTRACT Self‐healing polymers governed by supramolecular and dynamic covalent interactions are redefining structural design and functional integration in contemporary materials. Reversible supramolecular motifs, including hydrogen bonding and electrostatic interactions, enable rapid interfacial reconstruction and damage tolerance, whereas dynamic covalent bonds, such as Diels–Alder, disulfides, provide mechanically robust, reconfigurable, and recyclable network architectures. Their synergistic integration yields materials with repeatable healing, robust mechanics, and multimodal responsiveness. These advances have accelerated progress in flexible electronics, particularly capacitive sensing, where dedicated multilayer architectures, printable conductors, and minimal conductive dopants deliver enhanced sensitivity, a broad operational window, and rapid electrical and mechanical recovery; however, challenges such as scalable processing and property reconciliation remain unresolved. This review highlights recent advances in multifunctional dynamic polymer networks by delineating supramolecular and dynamic covalent self‐healing behaviors, their synergistic coupling, and their deployment in state‐of‐the‐art self‐healing sensor devices, providing insights for high‐performance flexible sensing technologies.