This work aimed to examine a permanent magnetic cation-exchange resin (MCER) for synergistic co-removal of Cu(II) and tetracycline (TC) from their mixed solutions. Batch adsorption experiments and characterizations were performed to elucidate the adsorption mechanisms. The adsorption of Cu(II) followed the Langmuir isotherm model in most cases, while Freundlich isotherm model was more suitable for fitting TC adsorption, which was due to the surface coordination between adsorbed Cu(II) and TC and the formation of multilayer MCER-Cu-TC complexes. The equilibrium TC adsorption amount in binary Cu/TC system was about 5.5-13.5 times of that in sole system, whereas Cu(II) uptake was nearly unchanged. Decomplexing-bridging was ascribed as the primary mechanism, which involved the [Cu-TC] decomplexing and [resin-Cu] bridging for TC uptake. Moreover, these MCER microbeads could be reused with negligible loss in adsorption capacity during five adsorption-desorption cycles, indicative of great potential in synergistic co-removal of organics-Cu complexes from aqueous solutions.