To address the urgent need for efficient removal of lead-containing wastewater and reduce the risk of toxicity associated with heavy-metal wastewater contamination, materials with high removal rates and easy separation must be developed. Herein, a novel organic-inorganic hybrid material based on phosphorylated magnetic chitosan (MSCP) was synthesized and applied for the selective removal of lead (II) from wastewater. From the characterization and the experimental results can be obtained that the magnetic saturation strength of MSCP reaches 14.65 emu/g, which can be separated quickly and regenerated readily, and maintains high adsorption performance even after 5 cycles, indicating that the adsorbent possesses good magnetic separation performance and durability. Also, MSCP showed high selective adsorption performance for lead in the multiple metal ions coexistence solutions at pH 6.0 and room temperature, with an adsorption coefficient SPb-MSCP of 78.85%, which was much higher than that of MSC (the SPb-MSC was 11.59%). Additionally, in the single lead system, the sorption characteristics of Pb(II) on MSCP and MCP had obvious pH-responsiveness, and their adsorption capacity increased with the increase of solution pH, reaching the maximal values of 80.19 and 72.68 mg/g, respectively. It is noteworthy that the acid resistance of MSCP with an inert layer coated on the core is significantly improved, with almost no iron leaching from MSCP over the entire acidity range, while MCP has 7.63 mg/g of iron leaching at pH 1.0. Significantly, MSCP exhibited a maximum adsorption capacity of 102.04 mg/g, which matches the Langmuir model at pH 6.0 and 298.15 K, and points to the pseudo-second-order kinetics of the chemisorption process of Pb(II) on MSCP. These findings highlight the great potential of MSCP for Pb(II) removal from aqueous solution, making it a promising solution for Pb(II) contamination in wastewater.