Variation of magnetic properties in two-dimensional (2D) thin films are extremely important for spintronic and data-storage applications, which has inspired scientists to design 2D devices that mimic their functions. We have effectively changed the magnetism and charge transfer in the new phases of 2D MnS2 bilayer. The underlying mechanism of the variation for magnetism and electronic structure are systemically analyzed. We show that our 2D bilayers with long-ranged antiferromagnetic (AFM) orders and stable magnetic easy axes belong to ideal semiconductors, where all the Mn ions are in high-spin states. Our bilayer provides a new platform for designing 2D magnetic thin films, which is beneficial to the application of MnS2 materials in data-storage and spintronic devices with low energy consumption, nonvolatility, and high-speed.