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Interlayer coupling is of vital importance for manipulating physicalproperties, e.g. electronic bandgap, in two-dimensional materials. However,tuning magnetic proper-ties in these materials is yet to be addressed. Here, wefound a striped antiferromag-netic (sAFM) to ferromagnetic (FM) transitionundergoing from monolayer to bilayer and thicker CrS2. This transition isattributed to charge sharing of interlayer S atoms and its resulting chargetransfer from Cr d eg to t2g orbitals. The transferred charge reduces a portionof Cr4+ to Cr3+, which enhances the double-exchange mechanism favoring FMrather than sAFM ordering. Doping of electrons shares the same effect withstacking induced charge sharing. Therefore, charge doping could eithermanip-ulate the magnetic ordering between sAFM and FM or tune CrS2 between p-and n-doped magnetic semiconductors. We also proposed several prototype devicesena-bling to use external electric field for manipulating magnetic orderings ofCrS2 layers. These results manifest the role of interlayer coupling inmodifying magnetic proper-ties of layered materials

Layer- and doping-tunable long range ferromagnetic order-ing in two-dimensional CrS2