TC4 alloy is widely used in dental implantation due to its excellent biocompatibility and low density. However, it is necessary to further improve the corrosion resistance and surface hardness of the titanium alloy to prevent surface damage that could result in the release of metal ions into the oral cavity, potentially affecting oral health. In this study, Ti-N-O layers were fabricated on the surface of TC4 alloy using a two-step hollow cathode plasma source oxynitriding technique. This resulted in the formation of TiN, Ti2N, TiO2, and nitrogen-stabilized α(N)-Ti phases on the TC4 alloy, forming a Ti-N-O modified layer. The microhardness of the samples treated with plasma oxynitriding (PNO) was found to be 300–400% higher than that of untreated (UN) samples. The experimental conditions were set at 520 °C, and the corrosion current density of the PNO sample was measured to be 7.65 × 10−8 A/cm2, which is two orders of magnitude lower than that of the UN sample. This indicates that the PNO-treated TC4 alloy exhibited significantly improved corrosion resistance in the artificial saliva solutions.