<p>Lightweight, homogeneously high-strength, and sustainable structural materials exert a crucial role in advanced engineering fields. Bamboo can be processed into high-performance structural material if its mechanical strength and homogeneity are remarkably enhanced. Herein, we report a strategy to process natural bamboo into a lightweight, robust, and durable structural material (HoRo-Bamboo) with homogenously high strengths in both longitudinal (L) and transversal (T) directions through bonding network reconstruction technology. The process requires the dispersion of fibers through H₂O₂/O₃ treatment, followed by the introduction of Al³⁺ and rapid pressing to reconstruct the ionic-hydrogen bonding network (IHBN). The as-prepared HoRo-Bamboo exhibits a low density of 0.83 g·cm⁻³ with superb high tensile strengths in both L (631 MPa) and T (628 MPa) directions, as well as the excellent environmental resistance and flame retardancy. Life cycle assessment shows that the carbon emissions from producing 1 kg of HoRo-Bamboo are 1.67 kg of CO₂ eq. Our approach enables bamboo to be an excellent alternative to existing structural materials, offering lightweight, super-robust, decarbonized, and sustainable features.</p>