We investigated the response times of eight volatile methylsiloxanes (VMSs) in environmental systems at different scales from local to global, with a particular focus on overall loss rates after cessation of emissions. In part, this is driven by proposals to restrict the use of some of these compounds in certain products in Europe. The GloboPOP model estimated low absolute Arctic Contamination Potentials for all VMSs and rapid response times in all media except sediment. VMSs are predicted to be distributed predominantly in air where they react with OH radicals, leading to short response times. After cessation of emissions VMSs concentrations in the environment are expected to decrease rapidly from current levels. Response times in specific water and sediment systems were evaluated using a dynamic QWASI model. Response times were sensitive to both physico-chemical properties and environmental characteristics. Degradation was predicted to play the most important role in determining response times in water and sediment. In the case of the lowest molecular weight VMSs such as L2 and D3, response times were essentially independent of environmental characteristics due to fast hydrolysis in water and sediment. However, response times for the other VMSs are system-specific. They are relatively short in shallow water bodies but increase with depth due to the diminishing role of volatilization on concentration change as volume to surface area ratio increases. In sediment, degradation and resuspension rates also contribute most to the response times. The estimated response times for local environments are useful for planning future monitoring programs.