Constructing a crystalline-amorphous hybrid structure is an effective strategy to overcome the conflict between the strength and toughness of materials. However, achieving such a material structure often involves complex, energy-intensive processing. Here, we leverage the natural wood featuring coexisting crystalline and amorphous regions to achieve superstrong and ultratough wood paper (W-paper) via a dual-phase nanostructure regulation strategy. After partially removing amorphous hemicellulose and eliminating most lignin, the treated wood can self-densify through an energy-efficient air drying, resulting in a W-paper with high tensile strength, toughness, and folding endurance. Coarse-grained molecular dynamics simulations reveal the underlying deformation mechanism of the crystalline and amorphous regions inside cell walls and the failure mechanism of the W-paper under tension. Life cycle assessment reveals that W-paper shows a lower environmental impact than commercial paper and common plastics. This dual-phase nanostructure regulation based on natural wood may provide valuable insights for developing high-performance and sustainable film materials.