ABSTRACT: Layered two-dimensional transition metal dichalcogenides, due to their semiconducting nature and large surface-to-volume ratio, have created their own niche in the field of gas sensing. Their large recovery time and accompanied incomplete recovery result in inferior sensing properties. Here, we report a composite-based strategy to overcome these issues. In this study, we report a facile double-step synthesis of a MoS2/SnO2 composite and its successful use as a superior room-temperature ammonia sensor. Contrary to the pristine nanosheet-based sensors, the devices made using the composite display superior gas sensing characteristics with faster response. Specifically, at room temperature (30° C), the composite-based sensor exhibited excellent sensitivity (10%) at an ammonia concentration down to 0.4 ppm along with the response and recovery times of 2 and 10 s, respectively. Moreover, the device also exhibited long-term durability, reproducibility, and selectivity toward ammonia against hydrogen sulfide, methanol, ethanol, benzene, acetone, and formaldehyde. Sensor devices made on quartz and alumina substrates with different roughnesses have yielded almost an identical response, except for slight variations in response and recovery transients. Further, to shed light on the underlying adsorption energetics and selectivity, density functional theory simulations were employed. The improved response and enhanced selectivity of the composite were explicitly discussed in terms of adsorption energy. Lowdin charge analysis was performed to understand the charge transfer mechanism between NH3, H2S, CH3OH, HCHO, and the underlying MoS2/SnO2 composite surface. The long-term durability of the sensor was evident from the stable response curves even after 2 months. These results indicate that hydrothermally synthesized MoS2/SnO2 composite-based gas sensors can be used as a promising sensing material for monitoring ammonia gas in real fields.