Within the last years, considerable progress was achieved in the research field of plasma nitriding of Al alloys. However, due to large property differences between the very hard AlN layer and the soft Al matrix material the load capacity of the nitride layer is limited. Electron beam (EB) surface alloying modifies the chemical composition of the area near the surface up to a certain depth. This, for instance, results in high hardness levels, and therefore this layer acts as support for the hard and wear-resistant thin AlN layer generated by plasma nitriding. In the present study, surface modifications produced by a combination of EB alloying with Fe based additives and plasma nitriding of wrought, cast and spray-formed Al alloys were investigated. After the EB treatment the layers were examined regarding their influence on the structure, the nitride layer growth mechanism, the effect of the EB layer for the support of the AlN layer and the resulting duplex layer properties, e.g. hardness and wear behaviour.