This paper reports the adsorption of toxic gases (NO 2 , SO 2 , and NH 3 ) on a MoSeTe structure based on first principles. It was found that the gas (NO 2 , SO 2 , and NH 3 ) adsorption on a pure MoSeTe monolayer was weak; however, the adsorption performance of these gas molecules on transitionmetal-atom-supported MoSeTe monolayers (TM−MoSeTe) was better than that on pure MoSeTe monolayers. In addition, there was more charge transfer between gas molecules and TM− MoSeTe. By comparing the adsorption energy and charge transfer values, the trend of adsorption energy and charge transfer in the adsorption of NO 2 and SO 2 was determined to be Fe−MoSeTe > Co−MoSeTe > Ni−MoSeTe. For the adsorption of NH 3 , the effect trend was as follows: Co−MoSeTe > Ni−MoSeTe > Fe− MoSeTe. Finally, by comparing their response times, the better gas sensor was selected. The Ni−MoSeTe system is suitable for NO 2 gas sensors, and the Fe−MoSeTe and Co−MoSeTe systems are suitable for SO 2 gas sensors. The Fe−MoSeTe, Co−MoSeTe, and Ni−MoSeTe systems are all suitable for NH 3 gas sensors. Janus transition-metal dichalcogenides have the potential to be used as gassensing and scavenging materials.