Efficient removal of Pb(II) and Cu(II) from wastewater is crucial for safeguarding environmental safety and public health. Biomass-based adsorbents with surface-specific functionality hold great promise for selective adsorption of metal cations. In this study, a novel phosphorylated chitosan-lignin (PCSL) composite is successfully synthesized via Mannich reaction. The PCSL exhibits remarkable selectivity in the adsorption of Pb(II) and Cu(II), as evidenced by Density Functional Theory (DFT) calculations. Furthermore, DFT analysis reveals that the incorporation of phosphate groups significantly enhances the chelation capacity of the adsorbent towards heavy metals. The PCSL demonstrates ultrafast adsorption capabilities for Pb(II) and Cu(II). Specifically, the adsorption processes reach equilibrium within 7 min and 5 min, respectively, with maximum adsorption capacities of 207.9 mg·g