As an advanced water purification technology, magnetic nanoabsorbents are highly attractive for their sustainability, robustness, and energy efficiency. However, magnetic responsiveness and high adsorptive capacity are irreconcilable during the design and synthesis of a high-performance magnetic nanoabsorbent. Here, we address this issue by designing a kind of mesoporous magnetic polymer hybrid microspheres, where functional polymers such as polyrhodanine and polypyrrole were attached to the pore walls in the interior of mesoporous Fe 3 O 4 microspheres through in situ polymerization. Due to the integrated large saturation magnetic moment, porous structure, and dense polymer layer, the mesoporous magnetic polymer hybrid microspheres demonstrated fast magnetic responsiveness, excellent recycling performance, and high adsorption capacities toward Pb(II) ions (189 mg g −1 ) for polyrhodanine and Cr(VI) ions (199 mg g −1 ) for polypyrrole. Furthermore, their potential application in wastewater treatment was verified by a self-made magnetic separation column, where the designed magnetic nanoabsorbent exhibits significant advantages including rapid separation of heavy metal ions and high outflow. This study provided a promising magnetic polymer hybrid nanoabsorbent for realizing efficient removal of heavy metal ions from wastewater.