very important parameters in their performance evaluation.Hydrogen sulfide H 2 S is a toxic gas that has hazardous effects on the respiratory system leading to neurological disorders as well. [1] H 2 S, also called sewer gas, is released during the decay of organic materials, septic systems during bacterial breakdown, and petroleum drilling and refining. Hence, the demand to investigate new functional materials for the detection of traces of H 2 S is quite relevant.Gas sensors have been fabricated using metal oxides, [6] polymers, [7,8] and organicinorganic hybrid materials [9][10][11] for the sensing of a particular analyte. Metal oxide based sensors, for example, SnO 2 , [2,12,13] TiO 2 , [14] and CuO/ZnO [15] are the most investigated since they exhibit high sensitivity, fast response, and recovery. However, they lack selectivity and possess safety and stability issues due to their high-temperature operation, [16,13] and the signal drift [17,18] with time hinders the integration and miniaturization of the devices. As possible alternatives to metal oxides, nanostructured metal sulfides (i.e., SnS 2 and Cu x S) [4,[19][20][21] and 2D layered transition metal dichalcogenides such as MoS 2 , [22] WS 2 , [23,24] and MoSe 2 [25,26] have been recently explored for NO 2 , NH 3 , and VOC sensing due to their tunable structural, electronic, and optical properties. Unfortunately, these materials are limited by their long response and recovery times and stability issues under ambient conditions. It has been reported that the decoration of noble metal nanoparticles (NPs) (Au, Ag, Pt) on metal oxides and metal sulfides enhances the performance of sensing materials in terms of their selectivity, stability, and recovery. [27] Nevertheless, this increases the cost and complexity of the synthesis and device fabrication.On the other hand, studies on the physical and chemical properties of metal chalcogenides have shown the competence of these materials to operate as sensors at low powers leading to conservation of energy and also from the safety point of view as they could be operated at low temperatures. [18] The relatively lower band gap of metal chalcogenides is an added advantage for application as compared to wide band gap of semiconductors. This motivates one to explore metal sulfides for sensing applications. [18] Several binary sulfides are used for sensing of gases such as NH 3 , NO 2 , and H 2 , but not for H 2 S, especially at room temperature, because of the relative inactivity of metal sulfide surface bonds for this gas. The situation can be entirely different in the ternary case, however, due to the possible synergy of interactions involving dual cation surface chemistry. This is borne out by the present work wherein the Cu 3 SnS 4 material, the Cu-rich ternary sulfide used for the first time in the gas sensing context, not only senses H 2 S at room temperature but also remarkably does so with high selectivity and stability. Thus, a combined experimental and computer modeling study on the use of nanocrystalline ort...