Low carbon steel substrates were covered with a ␥-glycidoxypropyltrimethoxysilane ͑␥-GPS͒ modified epoxy layer. Electrochemical impedance spectroscopy and attenuated total reflection infrared spectroscopy were used to investigate the barrier properties of the coating. The resistance of the samples to ion transport processes along the epoxy/steel interface was determined by in situ scanning Kelvin probe ͑SKP͒ measurements of the interface potential. X-ray photoelectron spectroscopy studies helped to analyze the resulting ion distribution on the substrate surface. The application of ␥-GPS resulted in a reduction of the interfacial water activity and temporarily stabilized the polymer/steel interface. In contrast to the experiments with the unmodified epoxy coating, interfacial ion transport processes were verifiable with the SKP. After some days of sample exposure to humid air, the stabilizing effect of ␥-GPS diminished and SKP potential profiles had to be recorded in dry atmosphere to identify the electrolyte front position, zones of cation and anion separation, and areas of local corrosion damage at the interface. This approach seems to be generally promising to analyze the degradation state of polymer/oxide/metal interfaces after long-term exposures in humid air.In Part I of this paper, the properties of a water-borne epoxy coating were analyzed. It was focused on the effect of high water activities and on the characteristics of ion transport processes at epoxy/steel interfaces. 1 Electrochemical impedance spectroscopy ͑EIS͒ indicated poor barrier properties of the polymer films. It was estimated that the H 2 O uptake level was very high and that strong wet adhesion processes occurred in humid air at the polymer/steel interface compared to substrates coated with common non-waterborne epoxy coatings. 2 Oxygen reduction induced ion transport processes along the epoxy/steel interface were not verifiable with the scanning Kelvin probe ͑SKP͒ because no characteristic sigmoid potential profiles were detected. Instead, the SKP recorded a nonspecific linear profile with a small slope. It was not possible to determine an electrolyte front position unless the humidity of the surrounding atmosphere was reduced. 1 Moreover, it was shown that both cations and anions of the defect electrolyte penetrated the epoxy/steel interface after the initialization of interfacial ion transport processes. With respect to previous studies, 3-9 it was discussed that the unexpected and uncommon anion transport was supported by the effects of fluid dynamics at the interface rather than by ion diffusion.This part of the study complements and continues the experimental approach selected in Part I. 1 It will be analyzed which effects a modification of the epoxy/steel interface with ␥-glycidoxypropyltrimethoxysilane ͑␥-GPS͒ has on the interface potentials and on the detectability of interfacial ion transport processes. Interfaces modified with adhesion promoting molecules, such as ␥-GPS, are expected to be more stable in an environment of a high ...