A new magnetically separable catalyst consisting of Cu(II) complex immobilized on Fe3O4 nanoparticles functionalized with diethylenetriamine (Fe3O4–DETA–Cu(II)) was successfully synthesized and characterized by FT-IR, SEM, EDS, VSM, TGA, XRD, and AAS techniques. This synthesized nanosolid was shown to be an efficient heterogeneous catalyst for the solvent-free synthesis of polyhydroquinoline derivatives. The catalyst was readily separated from the final product solution by magnetic decantation and reused for subsequent reactions for at least seven runs with less deterioration in catalytic activity.