Atomically thin layered materials such as MoS2 have future versatile applications in low power electronics. Here, we demonstrate the growth of a salt-assisted large scale, high-quality monolayer MoS2 toward the realization of a high-performance hysteresis-free field-effect transistor (FET). Density functional theory calculations are implemented to monitor the effects of the Schottky barrier and metal-induced gap states between our metal electrodes and MoS2 for achieving high carrier transport. The role of absorbed molecules and oxide traps on the hysteresis are studied in detail. For the first time, a hysteresis-free intrinsic transistor behavior is obtained by an amplitude sweep pulse I–V measurement with varying pulse widths. Under this condition, a significant enhancement of the field-effect mobility up to 30 cm2 V−1 s−1 is achieved. Moreover, to correlate these results, a single-pulse time-domain drain current analysis is carried out to unleash the fast and slow transient charge trapping phenomena. Our findings on the hysteresis-free transfer characteristic and high intrinsic field-effect mobility in salt-assisted monolayer MoS2 FETs will be beneficial for future device applications in complex memory, logic, and sensor systems.