Home health has become a global concern, as indoor environmental pollution poses a serious threat to human health. Traditional fiberboard used in interior decoration requires a large amount of adhesive, inevitably increasing costs and leading to pollution from harmful gases, such as formaldehyde and volatile organic compounds. The development of bamboo self-bonding products is a solution to the above-mentioned problems. The hydroxyl and carboxyl functional groups in bamboo can form cross-links through noncovalent interactions; however, these dynamic reversible noncovalent bonds are prone to breaking, leading to insufficient bonding strength. This study reports a dual-coordination network enhancement strategy for the preparation of self-bonding bamboo fiberboard (SBFB). Attributed to the enhanced noncovalent interactions of the COOH–Co2+–HOOC– and −OH–Co2+–HO– coordination networks, the SBFB has significantly higher hardness (shore hardness D 91.3) and flexural strength (92.3 MPa) than traditional fiberboard. In addition, the SBFB exhibits good plasticity. With the lubrication of water molecules, the glass-transition temperature of bamboo decreases from 227.6 to 53 °C, allowing the SBFB to be molded into any desired shape. The dual-coordination network enhancement strategy provides a feasible approach for the preparation of high-performance self-bonding biomass fiber materials.This study used sustainable bamboo fiber to fabricate a self-bonding bamboo fiber engineering material using a dual-coordination network enhancement strategy.