Renewable lignocellulosic materials are promising green plastic alternatives to fossil fuel-based plastics. However, the hydrophilic nature and poor water resistance of lignocellulosic materials have hindered their practical applications. This study reports a facile metal-ion-modification (MIM) route, swelling with aqueous metal ion solutions, and drying to convert conventional hydrophilic paper and wood pulp into biodegradable hydrophobic paper and tableware without the addition of hydrophobic sizing chemicals/materials. Metal ions such as Fe3+ and Zr4+ can coordinate with pulp fibers’ polar groups (i.e., O.H., C=O, and COOH) that induce self-assembly of their surface fibrillated “hairy” cellulose nanofibrils to form a more compact structure with fewer available O.H. groups for water sorption. The formation of coordination bonds with polar groups (i.e., O.H., C=O, and COOH) decreases the surface energy of pulp fibers and increases their hydrophobicity and water resistance. Only ~3 mg of metal ions is needed to induce the wettability transition in 1 g of kraft pulp, resulting in hydrophobic paper and tableware with water contact angles (WCAs) of 120-140° and displayed wet tensile strengths of up to 9.5 MPa, and low water absorbency, which were comparable to synthetic polymer films. This MIM technique can be integrated into the existing paper-making process for the scalable production of hydrophobic papers and tableware, providing an alternative route for developing sustainable and biodegradable plastic counterparts. The MIM-induced lignocellulose hydrophobization mechanisms were elucidated using X-ray photoelectron spectroscopy (XPS), Fourier transforms infrared spectroscopy (FT-IR), and scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS), and density functional theory (DFT). Furthermore, this MIM technique was also evaluated for its applicability in wood treatment. The treatment effectively tunes the wood surface from hydrophilic to hydrophobic, enhancing its water resistance. The MIM treatment significantly improved the dimensional stability of SYP, red oak, and poplar. For example, the Fe3+ treatment reduced the tangential swelling of SYP, poplar, and red oak by 57%, 50%, and 40%, respectively. Overall, this eco-friendly and facile MIM method holds promise for developing sustainable and biodegradable alternatives to conventional plastics, contributing to a more environmentally friendly future.

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