Emergence of Plasticity through Inter-Fibril Sliding in a Supramolecular Hydrogel

Abstract Biological matter consists of complex networks of fibrillar assemblies that can withstand substantial mechanical stress without brittle fracture. Replicating these properties in synthetic materials - particularly the combination of strain stiffening and structural plasticity - has remained challenging without relying on covalent polymers or permanent chemical crosslinking. Here we report a purely supramolecular hydrogel that uniquely integrates both strain stiffening and structural plasticity, and we introduce a multiscale framework for studying plasticity in supramolecular materials. The material incorporates two orthogonal interaction modes, physical crosslinks that drive strain-stiffening behaviour, and inter-fibril sliding that enables plastic deformation without loss of elastic stiffness. This work reveals structural plasticity as an emergent and designable property of supramolecular networks, opening routes toward bioinspired, adaptive soft matter beyond the elastic regime.