High-performance all-cellulose composites bulks enabled by a surface dissolution-intense shear plasticization...

All-cellulose composites (ACC) materials, where cellulose acts as both the reinforcement and matrix, possess high mechanical properties and biodegradability, positioning them as promising candidates for replacing petroleum-based plastics. However, fabricating robust ACC structural components remains challenging due to the processing challenges arising from its strong inter- and intramolecular interactions. To address this, a plasticization strategy based on surface dissolution-intense shear is proposed to fabricate high-performance ACC films and bulks. In this process, ionic liquids as solvents and intense shear force from a twin-roller mixer synergistically disrupt strong molecular interactions, achieving uniform surface dissolution even at a cellulose content as high as 60 wt%. Morphological and crystal evolution of cellulose during processing are characterized, and processing windows of ACC bulks using the layer-by-layer method are established. Mechanical results reveal that the tensile strength of ACC films reaches up to 98.20 ± 6.60 MPa, and the flexural strength and modulus of ACC bulk laminates reach over 100 MPa and 9 GPa, alongside complete biodegradability. This study provides a novel and efficient strategy for manufacturing biodegradable, high-performance structural components from sustainable resources.