© 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim A MoS2/graphene hybrid aerogel synthesized with two-dimensional MoS2 sheets coating a high surface area graphene aerogel scaffold is characterized and used for ultrasensitive NO2 detection. The combination of graphene and MoS2 leads to improved sensing properties with the graphene scaffold providing high specific surface area and high electrical and thermal conductivity and the single to few-layer MoS2 sheets providing high sensitivity and selectivity to NO2. The hybrid aerogel is integrated onto a low-power microheater platform to probe the gas sensing performance. At room temperature, the sensor exhibits an ultralow detection limit of 50 ppb NO2. By heating the material to 200 °C, the response and recovery times to reach 90% of the final signal decrease to <1 min, while retaining the low detection limit. The MoS2/graphene hybrid also shows good selectivity for NO2 against H2 and CO, especially when compared to bare graphene aerogel. The unique structure of the hybrid aerogel is responsible for the ultrasensitive, selective, and fast NO2 sensing. The improved sensing performance of this hybrid aerogel also suggests the possibility of other 2D material combinations for further sensing applications.