The construction of multinuclear lanthanide-based molecules with significant magnetic exchange interactions represents a key challenge in the realization of single-molecule magnets with high operating temperatures. Here, we report the synthesis and magnetic characterization of two series of heterobimetallic compounds, (Cp* 2 Ln) 2 (μ-Co(pdt) 2 ) (Ln = Y 3+ , Gd 3+ , Dy 3+ ; pdt 2− = 1,2-diphenylethylenedithiolate) and [K(18-crown-6)][(Cp* 2 Ln) 2 (μ-Co(pdt) 2 )] (Ln = Y 3+ , Gd 3+ ), featuring two lanthanide centers bridged by a cobalt bis(1,2dithiolene) complex. Dc magnetic susceptibility data collected for the Gd congeners indicate significant Gd−Co ferromagnetic exchange interactions with fits affording J = +11.5 and +7.33 cm −1 , respectively. Magnetization decay and ac magnetic susceptibility measurements carried out on the single-molecule magnet (Cp* 2 Dy) 2 (μ-Co(pdt) 2 ) reveal full suppression of quantum tunneling and open-loop hysteresis persisting up to 3.5 K. These results, along with those of high-field EPR spectroscopy, suggest that transition metalloligands can enforce strong exchange interactions with adjacent lanthanide centers while maintaining a geometry that preserves molecular anisotropy. Furthermore, the magnetic properties of [K(18-crown-6)][(Cp* 2 Gd) 2 (μ-Co(pdt) 2 )] show that increasing the spin of the ground state of the bridging complex may be a viable alternative to increasing J in obtaining well-isolated, strongly coupled magnetic ground states.