The Melanesian Volcanic Arc (MVA) emits about 12 kT d− 1 of sulfur dioxide (SO2) to the atmosphere from continuous passive (non-explosive) volcanic degassing, which contributes 20% of the global SO2 emission from volcanoes. Here we assess, from up-to-date and long-term observations, the SO2 emission of the Ambrym volcano, one of the dominant volcanoes in the MVA, and we investigate its role as sulfate precursor on the regional distribution of aerosols, using both satellite observations and model results at 1° × 1° spatial resolution from WRF-Chem/GOCART. Without considering aerosol forcing on clouds, our model parameterizations for convection, vertical mixing and cloud properties provide a reliable chemical weather representation, making possible a cross-examination of model solution and observations. This preliminary work enables the identification of biases and limitations affecting both the model (missing sources) and satellite sensors and algorithms (for aerosol detection and classification) and leads to the implementation of improved transport and aerosol processes in the modeling system. On the one hand, the model confirms a 50% underestimation of SO2 emissions due to satellite swath sampling of the Ozone Monitoring Instrument (OMI), consistent with field studies. The OMI irregular sampling also produces a level of noise that impairs its monitoring capacity during short-term volcanic events. On the other hand, the model reveals a large sensitivity on aerosol composition and Aerosol Optical Depth (AOD) due to choices of both the source function in WRF-Chem and size parameters for sea-salt in FlexAOD, the post-processor used to compute offline the simulated AOD. We then proceed to diagnosing the role of SO2 volcanic emission in the regional aerosol composition. The model shows that both dynamics and cloud properties associated with the South Pacific Convergence Zone (SPCZ) have a large influence on the oxidation of SO2 and on the transport pathways of volcanic species across the South Pacific atmosphere. For example, in the tropical cloudy air, the sulfate production in the aqueous phase is very efficient, resulting in the formation of a large cloud of highly scattering sulfate aerosols advected horizontally to Eastern Indonesia, in agreement with the AOD feature captured by MODIS/Aqua, but missed in CALIOP/CALIPSO (lidar) products. Model sensitivity experiments indicate that aerosol re-suspension due to evaporating droplets is a significant pathway for the supply of volcanic sulfur species in the remote marine boundary layer. By strongly modulating the irreversible loss due to wet scavenging, this aerosol process has a similar influence on the sulfur burden as natural emission from volcanoes or biogenic sources like dimethyl sulfate (DMS). The results emphasize the importance of MVA passive degassing and SPCZ dynamics on the aerosol background, and raise questions about potential impacts on the local climate and marine ecosystems.