A better understanding of degassing processes at open-vent basaltic volcanoes requires collection of new datasets of H2O–CO2–SO2 volcanic gas plume compositions, which acquisition has long been hampered by technical limitations. Here, we use the MultiGAS technique to provide the best-documented record of gas plume discharges from Stromboli volcano to date. We show that Stromboli's gases are dominated by H2O (48–98 mol%; mean, 80%), and by CO2 (2–50 mol%; mean, 17%) and SO2 (0.2–14 mol%; mean, 3%). The significant temporal variability in our dataset reflects the dynamic nature of degassing process during Strombolian activity; which we explore by interpreting our gas measurements in tandem with the melt inclusion record of pre-eruptive dissolved volatile abundances, and with the results of an equilibrium saturation model. Comparison between natural (volcanic gas and melt inclusion) and modelled compositions is used to propose a degassing mechanism for Stromboli volcano, which suggests surface gas discharges are mixtures of CO2-rich gas bubbles supplied from the deep (N4 km) plumbing system, and gases released from degassing of dissolved volatiles in the magma filling the upper conduits. The proposed mixing mechanism offers a viable and general model to account for composition of gas discharges at all volcanoes for which petrologic evidence of CO2 fluxing exists. A combined volcanic gas-melt inclusion-modelling approach, as used in this paper, provides key constraints on degassing processes, and should thus be pursued further.