This study investigated the potential application of an efficient, easily recoverable, and reusable copper(II)-based catalyst bearing polyvinyl alcohol (PVA) immobilized on FeNi3/KCC-1/APTPOSS [FeNi3/KCC-1/APTPOSS/TCT/PVA/Cu(II)] magnetic nano-particles (MNPs) for the N-formylation of amines via CO2 hydrogenation. FeNi3/KCC-1/TCT/PVA/Cu(II) MNPs were thoroughly characterized by transmission electron microscopy, field emission-scanning electron microscopy, vibrating sample magnetometry, thermo-gravimetric analysis, inductively coupled plasma-mass spectrometry (ICP-MS), and the Brunauer, Emmett, and Teller method. After the reaction, only minor changes to the morphology of the catalyst recycled by the ICP-MS were evidenced, thus corroborating its robustness.