Lignin as a Wood‐Inspired Binder Enabled Strong, Water Stable, and Biodegradable Paper for Plastic Replacement

Abstract Plastic waste has been increasingly transferred from land into the ocean and has accumulated within the food chain, causing a great threat to the environment and human health, indicating that fabricating an eco‐friendly and biodegradable replacement is urgent. Paper made of cellulose is attractive in terms of its favorable biodegradability, resource abundance, large manufacturing scale, and low material cost, but is usually hindered by its inferior stability against water and poor mechanical strength for plastic replacement. Here, inspired by the reinforcement principle of cellulose and lignin in natural wood, a strong and hydrostable cellulosic material is developed by integrating lignin into the cellulose. Lignin as a reinforced matrix is incorporated to the cellulose fiber scaffold by successive infiltration and mechanical hot‐pressing treatments. The resulting lignin‐cellulose composite exhibits an outstanding isotropic tensile strength of 200 MPa, which is significantly higher than that of conventional cellulose paper (40 MPa) and some commercial petroleum‐based plastics. Additionally, the composite demonstrates a superior wet strength of 50 MPa. Adding lignin also improves the thermostability and UV‐blocking performance of cellulose paper. The demonstrated lignin‐cellulose composite is biodegradable and eco‐friendly with both components from natural wood, which represents a promising alternative that can potentially replace the nonbiodegradable plastics.