The magneto-optic (MO) characteristics and sensing performance of noble metal (Ag, Au, Cu) or transition metal (Fe, Ni, Co) single layers and Ag/Co or Au/Co bilayers have been studied and compared in both the standard plasmonic and MO plasmonic configurations at two different wavelengths (632.8 nm and 785 nm) and in two different sensing media (air and water). The sensing performance is found to be medium-specific and lower in biosensor-relevant water-based media. The sensitivities of MO-SPR sensors is found to be superior to SPR sensors in all cases. This enhancement in sensitivity means the detection limit of this class of transducers can be substantially improved by tuning Au/Co layer thickness, wavelength, and incident angle of optical radiation. The optimized bilayer showed an enhancement in sensitivity by over 30× in air and 9× in water as compared to the conventional Au SPR configuration. Notably, the best performance is 3× above that of MO-SPR sensors coupled to a photonic crystal previously reported in the literature and is found when the ferromagnetic layer is furthest from the sensing medium, as opposed to typical MO-SPR configurations. This proposed structure is attractive for next-generation biosensors.