Reaction of an amphiphillic pentacyanoiron(III) complex with aqueous cobalt(II) ions at the air-water interface yielded a two-dimensional (2D) cobalt(II)-iron(III) cyanide network. The Langmuir monolayers were characterized by pressure vs. area isotherms. The cyanide-bridged networks were transferred to solid supports by the Langmuir-Blodgett technique. Multilayer films were structurally characterized by FT-IR and UV-VIS spectroscopies, X-ray diffraction and SQUID magnetometry.