Molybdenum disulfide (MoS2) is a representative two-dimensional layered transition-metal dichalcogenide semiconductor. Layer-number-dependent electronic properties are attractive in the development of nanomaterial-based electronics for a wide range of applications including sensors, switches, and amplifiers. MoS2field-effect transistors (FETs) have been studied as promising future nanoelectronic devices with desirable features of atomic-level thickness and high electrical properties. When a naturallyn-doped MoS2is contacted with metals, a strong Fermi-level pinning effect adjusts a Schottky barrier and influences its electronic characteristics significantly. In this study, we investigate multilayer MoS2Schottky barrier FETs (SBFETs), emphasizing the metal-contact impact on device performance via computational device modeling. We find thatp-type MoS2SBFETs may be built with appropriate metals and gate voltage control. Furthermore, we propose ambipolar multilayer MoS2SBFETs with asymmetric metal electrodes, which exhibit gate-voltage dependent ambipolar transport behavior through optimizing metal contacts in MoS2device. Introducing a dual-split gate geometry, the MoS2SBFETs can further operate in four distinct configurations:p - p,n - n,p - n, andn - p. Electrical characteristics are calculated, and improved performance of a high rectification ratio can be feasible as an attractive feature for efficient electrical and photonic devices.