Fe3O4‐supported copper (II) Schiff‐Base complex has been synthesized through post‐modification with 1,3‐phenylenediamine followed by further post‐modification with salicylaldehyde and coordination with Cu(II) ion. The resulted Fe3O4@SiO2‐imine/phenoxy‐Cu(II) magnetic nanoparticles (MNPs) were characterized by various techniques including SEM, TEM, XRD, XPS, EDX, VSM, FT‐IR, and ICP. The catalytic activity as a magnetically recyclable heterogeneous catalyst for one‐pot, three‐component synthesis of 2‐amino‐4H‐chromene derivatives was examined. The catalyst is efficient in the reaction and can be recovered by magnetic separation and recycled several times without significant loss in the catalytic activity.