Rapid urban industrialization and agricultural production have led to the discharge of excessive phosphate into aquatic systems, resulting in a rise in water pollution. Therefore, there is an urgent need to explore efficient phosphate removal technologies. Herein, a novel phosphate capture nanocomposite (PEI−PW@Zr) with mild preparation conditions, environmental friendliness, recyclability, and high efficiency has been developed by modifying aminated nanowood with a zirconium (Zr) component. The Zr component imparts the ability to capture phosphate to the PEI−PW@Zr, while the porous structure provides a mass transfer channel, resulting in excellent adsorption efficiency. Additionally, the nanocomposite maintains more than 80% phosphate adsorption efficiency even after ten adsorption–desorption cycles, indicating its recyclability and potential for repeated use. This compressible nanocomposite provides novel insights into the design of efficient phosphate removal cleaners and offers potential approaches for the functionalization of biomass−based composites.