By the reaction of the appropriate organometallic precursors and tetrakishydroxymethyl phosphonium chloride (THPC) at the toluene-water interface, we have prepared nanocrystalline films of Au-Ag and Au-Cu alloys with a range of compositions. The films have been characterized by X-ray diffraction, electron microscopy, optical spectroscopy, and other techniques, besides compositional analysis. The particle size of the nanocrystals in the films varies with the composition. The surface plasmon band of the alloy films as well as of the organosols obtained by the disintegration of the films by the addition of an alkanethiol show the expected composition dependence. It has been possible to prepare the nanocrystalline films of a ternary Au-Ag-Cu alloy.