The early stages of the formation of inorganic aggregates, composed of iron compounds at the solution-air interface, were investigated in situ. The properties of the solution-air interface were changed by using different Langmuir layers. In order to get insight into the evolution of the sample system in situ, the processes were studied by X-ray scattering and spectroscopy techniques. The formation of aggregates was detected under cationic as well as under anionic Langmuir layers. The observed compounds lack long range order which indicates the formation of amorphous structures. This is supported by extended X-ray absorption fine structure measurements showing only minor order in the formed aggregates.