Herein, we proposed a metal-ion-induced surface nano-engineering technology for transforming hydrophilic waste newspaper (WNP) into a hydrophobic material suitable for oil-water separation, without using hydrophobic chemicals/materials. WNPs were swelled in a dilute ferric ion solution (i.e., 50 mM FeCl3) followed by oven-drying to induce the coordination between ferric ions and hydroxyls of lignocellulose nanofibrils of the paper. This resulted in the crosslinking of lignocellulose nanofibrils and converted the hydrophilic WNP to the hydrophobic membrane (HM). The HM exhibited remarkable oil sorption capacity for various oils, up to 3.4 times its weight, and demonstrated good recyclability after undergoing 10 cycles of absorption-desorption-drying. Additionally, HM demonstrated the ability to effectively separate both immiscible oil-water mixtures and surfactant-stabilized water-in-oil emulsions in continuous gravity-driven oil-water separation processes. With the modification method and advantages in oil-water separation, the as-prepared HM exhibits great potential for application in oil spill treatment and environmental remediation.