In June 2019, the Raikoke volcano, Kuril Islands, emitted 0.4–1.8×109 kg of very fine ash and 1–2×109 kg of SO2 up to 14 km into the atmosphere. The eruption was characterized by several eruption phases of different duration and height summing up to a total eruption length of about 5.5 h. Resolving such complex eruption dynamics is required for precise volcanic plume dispersion forecasts. To address this issue, we coupled the atmospheric model system ICON-ART (ICOsahedral Nonhydrostatic with the Aerosols and Reactive Trace gases module) with the 1D plume model FPlume to calculate the eruption source parameters (ESPs) online. The main inputs are the plume heights for the different eruption phases that are geometrically derived from satellite data. An empirical relationship is used to derive the amount of very fine ash (particles <32 µm), which is relevant for long-range transport in the atmosphere. On the first day after the onset of the eruption, the modeled ash loading agrees very well with the ash loading estimated from AHI (Advanced Himawari Imager) observations due to the resolution of the eruption phases and the online treatment of the ESPs. In later hours, aerosol dynamical processes (nucleation, condensation, and coagulation) explain the loss of ash in the atmosphere in agreement with the observations. However, a direct comparison is partly hampered by water and ice clouds overlapping the ash cloud in the observations. We compared 6-hourly means of model and AHI data with respect to the structure, amplitude, and location (SAL method) to further validate the simulated dispersion of SO2 and ash. In the beginning, the structure and amplitude values for SO2 differed largely because the dense ash cloud leads to an underestimation of the SO2 amount in the satellite data. On the second and third day, the SAL values are close to zero for all parameters (except for the structure value of ash), indicating a very good agreement of the model and observations. Furthermore, we found a separation of the ash and SO2 plume after 1 d due to particle sedimentation, chemistry, and aerosol–radiation interaction. The results confirm that coupling the atmospheric model system and plume model enables detailed treatment of the plume dynamics (phases and ESPs) and leads to significant improvement of the ash and SO2 dispersion forecast. This approach can benefit the operational forecast of ash and SO2 especially in the case of complex and noncontinuous volcanic eruptions like that of Raikoke in 2019.