Strong Yet Tough Transparent Paper with Superb Foldability

Abstract Transparent paper manufactured from wood fibers is emerging as a promising, cost‐effective, and carbon‐neutral alternatives to plastics. However, fully exploring their mechanical properties is one of the most pressing challenges. In this work, a strong yet tough transparent paper with superior folding endurance is prepared by rationally altering the native fiber structure. Microwave‐assisted choline chloride/lactic acid deep eutectic solvent (DES) pulping is first utilized to isolate wood fibers from spruce wood. During this process, the S1 layer within the fibers is partially disrupted, forming protruding microfibrils that play a crucial role in enhancing cellulose accessibility. Subsequently, carboxymethylation treatment is applied to yield uniformly swollen carboxymethylated wood fibers (CM fibers), which improves the interaction between CM fibers during papermaking. The as‐prepared transparent paper not only shows a 90% light transmittance (550 nm) but also exhibits impressive mechanical properties, including a folding endurance of over 26 000, a tensile strength of 248.4 MPa, and a toughness of 15.6 MJ m⁻³. This work provides a promising route for manufacturing transparent paper with superior mechanical properties from wood fibers and can extend their use in areas normally dominated by high‐performance nonrenewable plastics.