The introduction of hydrogen-based energy production, storage, and conversion technologies requires materials that can withstand hydrogen's unique and reactive properties. A key concern is the durability of structural components, particularly issues like hydrogen embrittlement and corrosion in fuel cell and electrolyzer technologies. These factors are crucial as we transition to green and sustainable energy sources. Specifically, the interaction of hydrogen with the uppermost micrometers and the microstructural features of materials will significantly influence their performance. Thus, employing physical vapor deposition (PVD) coating materials to protect and enhance material surfaces will be essential for a wide range of future applications. Degradation mechanisms related to hydrogen occur at multiple length scales, involving different strategies for exposure or treatments. These strategies are typically divided into the two hydrogen-related material research worlds: (i) electrochemical degradation setups and (ii) and non-electrochemical treatments as a collective term for pressure/gas-related setups. Nevertheless, the broad field of hydrogen-related applications is increasingly merging. Consequently, the different degradation strategies primarily focus on electrochemical test setups as they are highly versatile. Therefore, in this study, the interaction of hydrogen with well-known protective coating materials such as TiN, CrN, ZrN, or TiAlN and AlCrN is described by an electrochemical Devanathan-Stachurski permeation setup. Different sets of these ceramic coating materials have been deposited on ferritic steel sheets through sputter and arc-evaporation technologies with varying deposition parameters. Subsequently, the coatings have been electrochemically loaded, and parameters such as diffusion coefficients, permeability, or permeation reduction factors are estimated. These results are correlated with the coatings’ microstructural appearance before and after hydrogen testing using a set of diverse high-resolution techniques such as SEM, TEM, XRD, and micro-mechanical testing methods.