Fe3O4 magnetic nanoparticles were prepared by hydrothermal synthesis and their surface was modified by the sol-gel method. Polymers imprinted with magnetic Cr (VI) were prepared by using Cr2O72- as template ion, 4-vinyl pyridine (4-VP) as monomer, isopropanol as solvent and Fe3O4 as matrix. The effects of solvent type, amount of Cr (VI) addition and volume of crosslinking agent on the adsorption properties of the imprinted polymers were investigated. The polymers were characterized by Fourier transform infrared (FT-IR) spectroscopy, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA). The adsorption equilibrium was reached within 50 min, and the maximum adsorption capacity was 201.55 mg·g-1. The adsorption process conformed to the Langmuir model, and the results of kinetic fitting showed that the pseudo-first-order kinetic model applied. In the Cr2O72-/AlF4- and Cr2O72-/CrO42- competitive systems, the imprinted polymer showed good selectivity to the template ions, with relative selectivity factors of 6.91 and 5.99, respectively. When the imprinted polymer was reused 6 times, the adsorption capacity decreased by only 8.2%, demonstrating good reusability.