The continuous reduction of magnetic units to ultrasmall length scales inspires efforts to look for a suitable means of controlling magnetic states. In this study, we show two surface charge alteration techniques for tuning the interlayer exchange coupling of ferromagnetic layers separated by paramagnetic spacers. Our ab initio study reveals that already a modest amount of extra charge can switch the mutual alignment of the magnetization from antiferromagnetic to ferromagnetic or vice versa. We also propose adsorption of alkali metals as an alternative way of varying the electronic and chemical properties of magnetic surfaces. Clear evidence is found that the interlayer magnetic order can be reversed by adsorbing alkalimetals on the magnetic layer. Moreover, alkali-metal overlayers strongly enhance the perpendicular magnetic anisotropy in FePt thin films. These findings combined with atomistic spin model calculations suggest that the electronic or ionic way of surface charging can have a crucial role for magnetic hardening and spin state control.