Single crystalline Ag/Fe/Fe0.5Co0.5/MgO(001) films were grown by Molecular Beam Epitaxy and investigated by Magneto-Optic Kerr Effect (MOKE). We find that even though the 4-fold magnetic anisotropies of Ag/Fe/MgO(001) and Ag/Fe0.5Co0.5/MgO(001) films are different from the corresponding bulk values, their opposite signs allow a fine tuning of the 4-fold magnetic anisotropy in Ag/Fe/Fe0.5Co0.5/MgO(001) films by varying the Fe and Fe0.5Co0.5 film thicknesses. In particular, the critical point of zero anisotropy can be achieved in a wide range of film thicknesses. Using Rotational MOKE, we determined and constructed the anisotropy phase diagram in the Fe and Fe0.5Co0.5 thickness plane from which the zero anisotropy exhibits a linear relation between the Fe and Fe0.5Co0.5 thickness
