Here, we demonstrate the impact of ferromagnetic layer coating on controlling the magneto-optical response. We found that the transverse magneto-optical Kerr effect (TMOKE) signal and TMOKE hysteresis loops of Ni80Fe20 thin layers coated with a Cr layer show a strong dependence on the thickness of the Cr layer and the incidence angle of the light. The transmission and reflection spectra were measured over a range of incidence angles and with different wavelengths so as to determine the layers’ optical parameters and to explain the TMOKE behavior. The generalized magneto-optical and ellipsometry (GMOE) model based on modified Abeles characteristic matrices was used to examine the agreement between the experimental and theoretical results. A comprehensive theoretical and experimental analysis reveals the possibility to create a TMOKE suppression/enhancement coating at specific controllable incidence angles. This has potential for applications in optical microscopy and sensors.