The aim of the present work is to study the CrN single‐layer coating and the Cr/CrN nanolayered coating by cathodic arc evaporation physical vapor deposition (CAE‐PVD) on AISI 304 stainless steel and to assess the electrochemical behavior of the coatings. Field emission scanning electron microscopy (FE‐SEM) and X‐ray diffraction (XRD) were utilized to study the morphology and microstructure of the coatings. The mechanical behavior of the coatings was studied by the nanoindentation technique. The electrochemical behavior of the formed coatings in 3.5 wt.% NaCl solution was investigated via electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization (PDP) tests. Based on the microscopic images, it was realized that both CrN and Cr/CrN coatings were formed having a dense structure on the substrate. The results of EIS measurements showed gradual changes in the polarization resistance of the Cr/CrN nanolayered coating during the immersion time. However, significant changes in the polarization resistance of the CrN single‐layer coating were seen by increasing immersion time comparing with the Cr/CrN coating. The higher polarization resistance of the Cr/CrN coating can be attributed to the effects of the interface between the layers in comparison to the CrN coating.