The ultrahigh surface-to-volume ratio and expandable interlayer spacing of van der Waals solids allow their channel bodies to strongly and dynamically interact with foreign molecules. However, controlling such multiple molecular interactions within a single, integrated platform has remained a technical challenge. Herein, we introduce a so-called hybrid-dual-gated voltage-controlled bimodal switch demonstrated on a single MoS2 transistor by cointegrating high-k solid and ionic liquid electrolytes as dual-gate dielectrics. Upon applying the synchronized dual-gate voltages, it results in two distinctive yet interchangeable switching modes: electrostatic near-Boltzmann-limit switching and intercalation-driven metal-insulator transitions. In addition to the improved field-effect switching performances (I on/I off similar to 109, SSmin similar to 61 mV/dec) in the low-gate voltage (V G) regime, the steep-slope metal-insulator transitions accompanying 2H-to-1T structural alternations can also be achieved in the high-V G regime. By incorporating conformal electrode passivation and independent dual-gating modulation, the proposed device platform enables highly stable, field-tunable bimodal switching behaviors through broad-range host-guest interactions.