For the first time, new hybrid organic-inorganic materials containing ferri-ferrocyanide and having a well-defined multilayer architecture were successfully obtained using the Langmuir-Blodgett (LB) technique. These LB films present a ferromagnetic behavior below 5.7 K. In this temperature range, their magnetic properties are clearly anisotropic, as expected from the lamellar structure. Finally, they are the first case of a new series of lamellar materials in which the magnetic properties of the inorganic sheets can be combined with other functions arising from the amphiphilic part.