The unique properties of MoS2 nanosheets make them a promising candidate for high-performance room temperature gas detection. Herein, few-layer MoS2 nanosheets (FLMN) prepared via mechanical exfoliation are coated on a substrate with interdigital electrodes for room-temperature NO2 detection. Interestingly, compared with other NO2 gas sensors based on MoS2, FLMN gas sensors exhibit high responsivity for room-temperature NO2 detection, and NO2 is easily desorbed from the sensor surface with an ultrafast recovery behavior, with recovery times around 2 s. The high responsivity is related to the fact that the adsorbed NO2 can affect the electron states within the entire material, which is attributed to the very small thickness of the MoS2 nanosheets. First-principles calculations were carried out based on the density functional theory (DFT) to verify that the ultrafast recovery behavior arises from the weak van der Waals binding between NO2 and the MoS2 surface. Our work suggests that FLMN prepared via mechanical exfoliation have a great potential for fabricating high-performance NO2 gas sensors.