Strong, Supertough and Self‐Healing Biomimetic Layered Nanocomposites Enabled by Reversible Interfacial Polymer Chain Sliding

Abstract Despite the remarkable progress in ultrastrong mechanical laminate materials, the simultaneous achievement of toughness, stretchability and self‐healing properties in biomimetic layered nanocomposites remains a great challenge due to the intrinsic limitations of their hard essences and lack of effective stress transfer at the organic‐inorganic fragile boundary. Here, an ultratough nanocomposite laminate is prepared by constructing chain‐sliding cross‐linking at the interface between sulfonated graphene nanosheets and polyurethane layers based on the ring molecules sliding on the linear polymer chains to release stresses. Unlike traditional supramolecular bonding toughening with limited sliding spacing, our strategy enables interfacial molecular chains reversible slippage when the inorganic nanosheets bear stretching force, providing sufficient interlayer spatial distance for relative sliding to dissipate more energy. The resulting laminates exhibit strong strength (22.33 MPa), supertoughness (219.08 MJ m −3 ), ultrahigh stretchability (>1900 %) and self‐healing ability (99.7 %), which far surpass most of reported synthetic and natural laminate materials. Moreover, the fabricated proof‐of‐concept electronic skin shows excellent flexibility, sensitivity and healability for human physiological signals monitoring. This strategy breaks through the challenge that traditional layered nanocomposites are intrinsically stiff and opens up the functional application of layered nanocomposites in flexible devices.