High-performance, fast-growing natural materials with sustainable and functional features currently arouse significant attention. Here, facile processing, involving delignification, in situ hydrothermal synthesis of TiO2 and pressure densification, is employed to transform natural bamboo into a high-performance structural material. The resulting TiO2-decorated densified bamboo exhibits high flexural strength and elastic stiffness, with both properties more than double that of natural bamboo. Real-time acoustic emission reveals the key role of the TiO2 nanoparticles in enhancing the flexural properties. The introduction of nanoscale TiO2 is found to markedly increase the degree of oxidation and the formation of hydrogen bonds in bamboo materials, leading to extensive interfacial failure between the microfibers, a micro-fibrillation process that results in substantial energy consumption and high fracture resistance. This work furthers the strategy of the synthetic reinforcement of fast-growing natural materials, which could lead to the expanded applications of sustainable materials for high-performance structural applications
