Aligned Bacterial Cellulose through Organohydrogel Transformation.

Bacterial cellulose (BC) possesses exceptional intrinsic mechanical properties at the nanoscale; however, translating these properties to the macroscopic level remains challenging due to its disordered nanofibrillar network. While mechanical stretching can induce nanofibrillar alignment within BC hydrogel, conventional techniques often cause structural damage, limiting both stretchability and achievable mechanical properties. To address this issue, we introduce a simple, one-step method by developing a BC organohydrogel via glycerol infusion into the BC network. This transformation significantly improves stretchability while maintaining structural integrity, enabling effective nanofibril rearrangement and alignment. After drying, the stretched organohydrogel yields BC sheets with high tensile strength (∼377 MPa) and Young's modulus (∼34 GPa), while maintaining flexibility. Morphological and orientation analyses reveal progressive alignment, with calculated Hermans orientation factor increasing from 0.24 for the hydrogel to 0.48 for the stretched organohydrogel. This organohydrogel transformation offers a promising approach to developing high-performance cellulose for structural, packaging, and electronic applications.