Ultrahigh Tough, Super Clear, and Highly Anisotropic Nanofiber-Structured Regenerated Cellulose Films.

While tremendous efforts have been dedicated to developing environmentally friendly films made from natural polymers and renewable resources, in particular, multifunctional films featuring extraordinary mechanical properties, optical performance, and ordered nanostructure, challenges still remain in achieving all these characteristics in a single material via a scalable process. Here, we designed a green route to fabricating strong, super tough, regenerated cellulose films featuring tightly stacked and long-range aligned cellulose nanofibers self-assembled from cellulose solution in alkali/urea aqueous systems. The well-aligned nanofibers were generated by directionally controlling the aggregation of cellulose chains in the hydrogel state using a preorientation-assisted dual cross-linking approach; i.e., a physical cross-linking was rapidly introduced to permanently reserve the temporarily aligned nanostructure generated by preorienting the covalent cross-linked gels. After a structural densification in air-drying of hydrogel, high strength was achieved, and more importantly, a record-high toughness (41.1 MJ m) in anisotropic nanofibers-structured cellulose films (ACFs) was reached. Moreover, the densely packed and well-aligned cellulose nanofibers significantly decreased the interstices in the films to avoid light scattering, granting ACFs with high optical clarity (91%), low haze (<3%), and birefringence behaviors. This facile and high-efficiency strategy might be very scalable in fabricating high-strength, super tough, and clear cellulose films for emerging biodegradable next-generation packaging, flexible electronic, and optoelectronic applications.