Using a Langmuir-Blodgett (LB) synthesis method, novel two-dimensional (2D) mixed-spin magnetic systems, in which each magnetic layer is both structurally and magnetically isolated, have been generated. Specifically, a 2D Fe-Ni cyanide-bridged network with a face-centered square grid structure has been magnetically and structurally characterized. The results indicate the presence of ferromagnetic exchange interactions between the Fe$^{3+}$ ($S=1/2$) and Ni$^{2+}$ (S=1) centers.