First-principles calculations of the magnetocrystalline anisotropy energy have been performed and it is predicted that the perpendicular magnetic anisotropy energy of a Au/(Fe-Co)(111) multilayer will be lager than that of a Au/Co multilayer. This multilayer was then grown by MBE method and found to have the predicted properties. The surface magnetic anisotropy energy is 0.64 mJ/m2, which is larger than the value reported previously for the Au/Co multilayer by 10%. The result indicates the possibility to control the magnetic anisotropy by changing the bandfilling.