We describe the synthesis of a series of novel nitrogen- and phosphorus-enriched biochar (activated carbon, AC) nanocomposites via the co-pyrolysis of Camellia oleifera shells (COSs) with different weight ratios of ammonium polyphosphate (APP) (wAPP: wCOSs = 1–3:1). The physicochemical characteristics of these nanocomposites (APP@ACs) were investigated via X-ray diffraction (XRD), Raman spectroscopy, N2 adsorption/desorption analysis, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). The results revealed that the APP@ACs exhibited richer N- and P-containing functional groups than unmodified AC. In addition, the removal performance of APP@AC-3 with respect to Pb(II) (723.6 mg g−1) was greatly improved relative to unmodified AC (264.2 mg g−1). Kinetic and equilibrium data followed the pseudo-second-order kinetic model and Langmuir model, respectively. The removal mechanism could be attributed to partial physisorption and predominant chemisorption. The N2 adsorption/desorption isotherms demonstrated that pore-volume properties could be an effective physical trap for Pb(II). Furthermore, the XPS and FTIR analysis revealed that the chemical removal mechanism of the APP@ACs is surface complexation via N-containing and P-containing functional groups. These findings indicate that the co-pyrolysis of COSs and APP leads to the formation of nitrogen- and phosphorus-containing functional groups that facilitate excellent activated carbon-based (biochar) adsorption performance.