SAE 5160 steel, classified as high-strength, low-alloy steel, is widely used in the automotive sector due to its excellent mechanical strength and ductility. However, its inherently low corrosion resistance limits its broader application. This study explores the application of the cathodic cage plasma deposition (CCPD) technique to enhance the corrosion resistance of SAE 5160 steel. The treatment was performed using a Hastelloy cathodic cage under two atmospheric conditions: hydrogen-rich (75%H2/25%N2) and nitrogen-rich (25%H2/75%N2). Comprehensive analyses revealed significant improvements in surface properties and corrosion resistance. The hydrogen-rich condition (H25N) facilitated the formation of Cr0.4Ni0.6 and CrN phases, associated with a nanocrystalline structure (37.6 nm) and a thicker coating (45.5 μm), resulting in polarization resistance over 290 times greater than that of untreated steel. Conversely, nitrogen-rich treatment (H75N) promoted the formation of Fe3N and Fe4N phases, achieving a dense but thinner layer (19.6 μm) with polarization resistance approximately 20 times higher than that of untreated steel. These findings underscore the effectiveness of CCPD as a versatile and scalable surface engineering technique capable of tailoring the properties of SAE 5160 steel for use in highly corrosive environments. This study highlights the critical role of optimizing gas compositions and treatment parameters, offering a foundation for advancing plasma-assisted technologies and alloying strategies. The results provide a valuable framework for developing next-generation corrosion-resistant materials, promoting the longevity and reliability of high-strength steels in demanding industrial applications.