“…When developing such high-strength and tough structural materials, natural polymers should be preferred due to their renewable and sustainable characteristics [ 7 , 8 ]. Cellulose is the most abundant biopolymer on Earth, found in trees, bamboo, rattan, agricultural crops, and other biomass, even bacteria [ 9 , 10 , 11 , 12 , 13 , 14 ]. Cellulose possesses attractive intrinsic mechanical properties with tensile strength of about 3.0−4.7 GPa g −1 cm 3 and a theoretical modulus of about 63−125 GPa g −1 cm 3 in its crystal region [ 15 , 16 ], both of which are higher than most metals, alloys, and some ceramics, which makes it an ideal building block for a series of strong and tough materials, such as nanopaper, films, and superstrong wood [ 17 , 18 , 19 ].…”