We apply multimedia models to systematically evaluate the fate profile of cyclic volatile methyl siloxanes (VMS) D-4, D-5 and D-6, and the linear VMS L-4 and L-5 using recently reported measurements of their partition ratios between organic carbon and water (K-OC), their salting out constants (K-s), and their enthalpy of sorption to organic carbon (Delta H-OC). Our assessment follows a multi-stage strategy where the environmental fate of the chemicals is explored in generic regional models with increasing fidelity to the real system and in a region-specific model. Modeled emissions of VMS to air remained in air and were degraded or advected out of the system with overall residence times ranging from 2.4 to 2.5 days, while emissions to water resulted in accumulation in sediment and longer residence times ranging from 29.5 to 1120 days. When emitted to water the modeled residence times of VMS in the sediment exceeded the REACH criterion for persistence in freshwater sediments. Reported K-OC measurements for D-5 differ by 1 log unit, which results in a 500-day difference in the overall residence times calculated in the generic regional modeling. In the specific-region modeling assessment for Adventfjorden, Svalbard in Norway, the different K-OC measurements of D5 resulted in a 200-day difference in overall residence times. Model scenarios that examined combinations of previously published Delta H-OC or enthalpy of phase change between octanol and water (Delta H-OW) for D5 in combination with the range of the K-OC measurements resulted in 1100-days difference in overall residence times. Our results demonstrate that residence times of VMS in aquatic systems are highly sensitive to their degree of sorption to organic carbon, and that residence times of VMS likely exceed several persistence criteria and therefore they cannot be considered as non-persistent. Environmental significance Volatile methylsiloxanes (VMS) are a group of organosilicon chemicals that are used in personal care products and in the production of silicone polymers. VMS have been found at considerable levels in the air, in sediments and in aquatic organisms. We examine the fate of VMS using multimedia models in aquatic environments and we study their residence times in generic and specific environmental scenarios. Our calculations suggest that the residence times of VMS exceed several persistence criteria in aquatic environments and therefore they cannot be regarded as non-persistent chemicals.