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In this paper, a novel ion-imprinted electrochemical sensor modified with magnetic nanomaterial Fe₃O₄@SiO₂ was established for the high sensitivity and selectivity determination of UO₂²⁺ in the environment. Density functional theory (DFT) was employed to investigate the interaction between templates and binding ligands to screen out suitable functional binding ligand for the reasonable design of the ion imprinted sensors. The MIIP/MCPE (magnetic ion imprinted membrane/magnetic carbon paste electrode) modified with Fe₃O₄@SiO₂ exhibited a strong response current and high sensitivity toward uranyl ion comparison with the bare carbon paste electrodes. Meanwhile, the MCPE was fabricated simultaneously under the action of strong magnetic adsorption, and the ion imprinted membrane can be adsorbed stably on the electrode surface, handling the problem that the imprinted membrane was easy to fall off during the process of experimental determination and elution. Based on the uranyl ion imprinting network, differential pulse voltammetry (DPV) was adopted for the detection technology to realize the electrochemical reduction of uranyl ions, which improved the selectivity of the sensor. Thereafter, uranyl ions were detected in the linear concentration range of 1.0 × 10⁻⁹ mol L⁻¹ to 2.0 × 10⁻⁷ mol L⁻¹, with the detection and quantification limit of 1.08 × 10⁻⁹ and 3.23 × 10⁻¹⁰ mol L⁻¹, respectively. In addition, the sensor was successfully demonstrated for the determination of uranyl ions in uranium tailings soil samples and water samples with a recovery of 95% to 104%.