Abstract: A magnetic carbon-based lithium ion-imprinted material (Li⁺-IIP-Fe₃O₄@C) with a high Li⁺ adsorption selectivity was designed and prepared by a surface ion imprinting method, using magnetic carbon nanospheres (Fe₃O₄@C) as the carrier and 2-hydroxymethyl-12-crown-4 as the adsorption unit. First, Fe₃O₄@C was silanized by γ-methacryloxypropyltrimethoxysilane to obtain Si-Fe₃O₄@C which was then functionalized with methacrylic acid (MAA), followed by polymerization to obtain PMAA-Fe₃O₄@C with a regular morphology and a high degree of MAA grafting. Finally, 2-hydroxymethyl-12-crown-4 was grafted onto the surface of PMAA-Fe₃O₄@C in the presence of LiClO₄ under catalysis by p-toluenesulfonic acid. This was cross-linked by ethylene glycol dimethacrylate and eluted by a HNO₃ solution to obtain Li⁺-IIP-Fe₃O₄@C. The kinetic adsorption and isothermal adsorption results for this material show that the adsorption of Li⁺ conforms to a pseudo-second-order kinetic model and has Langmuir isotherms. The maximum adsorption capacity of Li⁺-IIP-Fe₃O₄@C for Li⁺ is 22.26 mg/g at 25 ℃. The selection factors of Li⁺ against Na⁺, K⁺ and Mg²⁺ are 8.06, 5.72, and 2.75, respectively. The Li⁺ adsorption capacity of Li⁺-IIP-Fe₃O₄@C decreases by only 8.8% after six adsorption-desorption cycles, demonstrating an excellent regeneration capability and making it very useful for lithium recovery.