We demonstrated the sensitivity enhancement for magneto-optical surface plasmon resonance (MOSPR) using noble/ferromagnetic metals multilayers. The proposed structure is based on the Kretschmann configuration in the transverse magneto-optical Kerr effect (TMOKE) methods with the FeCu superlattices (SLs) as magneto-plasmonic materials and gelatin as biomolecules analyte. The dielectric constants of the FeCu SLs are taken from first principles calculation, which is performed by using a full-potential linearized augmented plane wave (FLAPW) method. The important role of the hybridization process in optical transitions has been identified, and it can be modulated by adjusting the thickness of superlattices. The dependence of the reflectivity on the dielectric constant is performed by 4×4 transfer matrix methods. It is found that the minimum reflectivity directly influences the slope of angular spectra, with a maximum slope of TMOKE signal is 12.23/degree. The change in the gelatin’s refractive index results in TMOKE signal response, then the enhancement of the sensitivity of the MOSPR system can be shown.