Engine blocks of modern passenger car engines are generally made of light metal alloys, mostly hypoeutectic AlSi-alloys. Due to their low hardness, these alloys do not meet the tribological requirements of the system cylinder running surface—piston rings—lubricating oil. In order to provide a suitable cylinder running surface, nowadays cylinder liners made of gray cast iron are pressed in or cast into the engine block. A newer approach is to apply thermal spray coatings onto the cylinder bore walls. Due to the geometric conditions, the coatings are applied with specifically designed internal diameter thermal spray systems. With these processes a broad variety of feedstock can be applied, whereas mostly low-alloyed carbon steel feedstock is being used for this application. In the context of this work, an iron-based wire feedstock has been developed, which leads to a nanocrystalline coating. The application of this material was carried out with the Plasma Transferred Wire Arc system. AlMgSi0.5 liners were used as substrates. The coating microstructure and the properties of the coatings were analyzed.