Heterotopic ligands containing chemically different binding centers are appealing candidates for obtaining heteronuclear metal complexes. By exploiting this strategy, it is possible to introduce different paramagnetic centers characterized by specific anisotropic magnetic properties that make them distinguishable when weakly magnetically coupled. This molecular approach has great potential to yield multi-spin adducts capable of mimicking logical architectures necessary for quantum information processing (QIP), i.e., quantum logic gates. A possible route for including a single-ion magnetic center within a finite-sized heterometallic compound uses the asymmetric (1-pyridyl)-butane-1,3-dione (pybd) ligand reported in the literature for obtaining Cr3+−Cu2+ metallo-cages. To avoid the formation of cages, we adopted the cyclen (1,4,7,10-tetraazacyclododecane) ligand as a “capping” agent for the Cu2+ ions. We report here the structural and magnetic characterization of the unprecedented adduct {Cr(pybd)3[Cu(cyclen)]2}(BF4)4, whose structure is characterized by a central Cr3+ ion in a distorted octahedral coordination environment and two peripheral Cu2+ ions with square-pyramidal coordination geometries. As highlighted by Continuous Wave Electron Paramagnetic Resonance (EPR) spectroscopy and Direct Current (DC) magnetometry measurements, this adduct shows negligible intramolecular magnetic couplings, and it maintains the characteristic EPR signals of Cr3+ and Cu2+ moieties when diluted in frozen solutions.