With the aim of improving the protective properties of Ni-Mo alloy layers, pulse reverse electrodeposition has been investigated. The anodic pulses were applied in the potential range where hydrogen desorption and oxidation occur. The alloy composition was shown to depend on the pulse parameters, especially on the anodic pulse duration. For long anodic pulses a preferential dissolution of molybdenum in the electrodeposited alloy occurs, while bulk Ni-Mo alloys do not undergo any dissolution. For anodic pulses longer than a certain threshold the electrocrystallization process becomes blocked. The morphology and microstructure of the layers are mainly determined by the molybdenum content rather than by the pulse parameters.