Two-dimensional (2D) Janus transition-metal dichalcogenides (TMDs) (MXY, M ¼ Mo, W; X, Y ¼ S, Se, Te; X s Y) have desirable energy gaps and high stability in ambient conditions, similar to traditional 2D TMDs with potential applications in electronics. But different from traditional 2D TMDs, 2D Janus TMDs possess intrinsic Rashba spin splitting due to out-of-plane mirror symmetry breaking, with promising applications in spintronics. Here we demonstrate a new and effective way to manipulate the Rashba effect in 2D Janus TMDs, that is, charge doping, by using first-principles density functional theory (DFT) calculations.We find that electron doping can effectively strengthen the Rashba spin splitting at the valence band maximum (VBM) and conduction band minimum (CBM) in 2D Janus TMDs without constant energy consumption, superior to traditional techniques (electric fields and strain engineering), but hole doping would weaken the Rashba effect in 2D Janus TMDs. By combining the DFT calculations with the electric-triple-layer model, we also reveal the intrinsic mechanism of tuning the Rashba effect in 2D Janus TMDs by charge doping, and find that the charge transfer plays an important role in tuning the Rashba spin splitting in 2D polar semiconductors. In particular, the Rashba constants are linearly dependent on the charge transfer between X (or Y) and M atoms in 2D Janus TMDs. These results enrich the fundamental understanding of the Rashba effect in 2D semiconductors, which can be promising candidates for spin field-effect transistors (FETs) in experiments. Recently, a polar TMD monolayer, MoSSe, has been successfully synthesized in experiments, 17,18 and is a Janus TMD. 2D Janus TMD monolayers MXY (M ¼ Mo, W; X, Y ¼ S, Se, Te; X s Y) show desirable energy gaps (1.0-2.0 eV) 19,20 and high stability [17][18][19][20] in ambient conditions, similar to traditional 2D TMDs 21-23 with potential applications in electronics. In particular, the Janus TMD monolayers show intrinsic Rashba spin splitting due to the