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Metal-organic frameworks (MOFs) with systematically tailored structures have been suggested as promising precursors to the preparation of diverse functional materials. Herein, a facile and versatile layer-by-layer strategy without any special surface modifications has been proposed for the preparation of magnetic metal-organic frameworks (MMOFs) supported molecularly imprinted polymer nanoparticles (MMOFs@MIP), which are based on a magnetically susceptible core conjugated with an imidazole-derived self-assembled layer and a silane-based imprinted shell. The obtained MMOFs@MIPs, which integrated the advantages of Fe₃O₄, MOFs, and MIPs, were characterized and exhibited good magnetic properties, a rapid mass transfer rate, and an excellent adsorption selectivity as well as capacity for the targeted molecular - bisphenol A (BPA). Moreover, the MMOFs@MIPs were employed as adsorbents in magnetic solid phase extraction (MSPE) to selectively bind and rapidly separate BPA from real samples with satisfactory recoveries ranging from 88.3% to 92.3%. More importantly, the desirable reusability of MMOFs@MIP was also evaluated, and the recoveries still maintained above 88.0% even after five re-use cycles. Furthermore, combined with high-performance liquid chromatography (HPLC) analysis, a novel MSPE-HPLC method was developed, enabling the highly selective and sensitive detection of BPA in a wide linear range of 0.5–5000 μg L⁻¹ with a low limit of detection (LOD) of 0.1 μg L⁻¹. This work contributes a promising method for constructing various functional nanoparticles @MOFs@MIP hybrid materials for applications in many different fields.