Lead (Pb) pollution has triggered a great threat to ecological system as well as public health due to its highly toxic and mutagenic properties. In this study, chitosan surface modified persimmon tannin (PT-CS) biomass composite as an environmental-friendly bioadsorbent for highly efficient removal of Pb(II) from aqueous solutions was investigated. Fourier-transform infrared spectroscopy, X-ray diffraction, scanning electron microscope, Brunauer–Emmett–Teller, X-ray photoelectron spectroscopy and Zeta potential were used to elucidate the adsorption mechanism. Combining oxidation reaction, electrostatic interaction and chelation reaction, PT-CS exhibited fine adsorption to Pb(II). The maximum adsorption capacity was 179.3 mg/g. Equilibrium isotherm for the adsorption of Pb(II) was analyzed by the Langmuir, Freundlich and Temkin models, and the Langmuir isotherm (R² > 0.99) was the best. The pseudo-first-order, pseudo-second-order and intraparticle diffusion equations were used to analyze the kinetic data of the adsorption process and the pseudo-second-order kinetic (R_s² > 0.98) model was fitted well. Moreover, thermodynamic parameters including ΔG⁰< 0, ΔH⁰ (150.57 KJ/mol) > 0 and ΔS⁰ (456.13 J/mol K) > 0 showed that the process of Pb(II) adsorption by PT-CS was spontaneous and endothermic. All these results illustrated that PT-CS would be a promising and low-cost alternative bioadsorbent of Pb(II) in wastewater treatment.