Surface condition and corrosion resistance are major concerns when metallic materials are going to be utilized for applications. In this study, FeCoNiCr medium-entropy alloy (MEA) is first treated with a nitrogen atmospheric-pressure plasma jet (APPJ) and then coated with octadecyltrichlorosilane (OTS) for the surface modification. The hydrophobicity of the FeCoNiCr MEA was effectively improved by OTS-coating treatment, APPJ treatment, or the combination of both treatments (OTS-coated APPJ-treated), which increased the water contact angle from 54.49° of the bare MEA to 70.56°, 93.94°, and 88.42°, respectively. Potentiodynamic polarization and electrochemical impedance spectroscopy tests demonstrate that the APPJ-treated FeCoNiCr MEA exhibits the best anti-corrosion properties. X-ray photoelectron spectroscopy reveals that APPJ treatment at 700 °C oxidizes all the alloying elements in the FeCoNiCr MEA, which demonstrates that a short APPJ treatment of two-minute is effective in forming a metal oxide layer on the surface to improve the corrosion resistance of FeCoNiCr MEA. These results provide a convenient and rapid method for improving surface properties of FeCoNiCr MEA.