Ternary Supramolecular Ensembles of Cellulose Nanocrystals Exhibiting Multiscale Deformation and Mechano/Chemoresponsive Selective Reflection of Circularly Polarized Light

Strong and tough structural materials are a challenging materials engineering problem that has drawn considerable attention among the materials community. Here we demonstrate that ternary supramolecular ensembles of cellulose nanocrystals-polyvinyl alcohol-glucose by evaporation-induced corporative assembly achieved simultaneous enhancement on the stiffness and toughness with the Young’s modulus of 13 GPa at the work-of-fracture of 1.1 MJ·m–3. Compositional alteration led to stiff and tough ternary ensembles with the Young’s modulus up to 14.7 GPa and the toughness up to 12.1 MJ·m–3, respectively. Concurrent enhancement in the stiffness and toughness was owing to the multiscale deformation involving weak interactions and helicoidal organization, leading to more efficient energy dissipation. The freestanding transparent films of the ternary ensembles exhibited dynamic selective reflection of left-handed circularly polarized light in response to mechanical and chemical stimuli. The combination of the mechanical, chemical, and sustainability-linked advantages with the stimuli-responsive selective reflection of circularly polarized light renders the ternary ensembles promising potentials as an implant for remote monitoring of mechanical strain and as a camouflaging material for security applications.