Transformation of Bamboo: From Multiscale Fibers to Robust and Degradable Cellulose‐Based Materials for Plastic Substitution

Abstract Bamboo is an ideal candidate to replace traditional plastics, reduce environmental pollution, and promote harmony between nature and humanity owing to its rapid growth and renewability. However, achieving arbitrary shape‐shifting of bamboo while retaining its high strength and degradability remains challenging. This study uses multiscale interface engineering to transform bamboo into a robust, biodegradable, and moldable bamboo cellulose‐based material. First, natural bamboo is deconstructed into cellulose fibers, including macro‐ and nanofibers. Subsequently, the fibers are constructed into high‐performance materials using physical and chemical methods, such as surface charge treatment, ion cross‐linking, and dense hydrogen bonding networks. The prepared multiscale bamboo cellulose‐based materials exhibit excellent properties, with a high specific strength (≈271.8 kN m kg −1 ), high impact toughness (≈58 kJ m −2 ), low thermal expansion coefficient (1.19 × 10 −6 K −1 ), excellent formability and biodegradability, and minimal environmental impacts. These properties are superior to those of current commercial plastics and other biomass‐derived structural materials. Furthermore, the mechanical properties of the materials can be customized by adjusting the layup configuration, enabling a transition from anisotropic to isotropic characteristics. This transformation demonstrates the significant potential of bamboo for plastic substitution and advances the development of environmentally friendly materials.