Rhyolitic eruptions beneath Icelandic glaciers can be highly explosive, as demonstrated by Quaternary tephra layers dispersed throughout northern Europe. However, they can also be small and effusive. A subglacial rhyolitic eruption has never been observed, so behavioral controls remain poorly understood and the influence of pre-eruptive volatile contents is unknown. We have therefore used secondary ion mass spectrometry to characterize pre-eruptive volatile contents and degassing paths for five subglacial rhyolitic edifices within the Torfajökull central volcano, formed in contrasting styles of eruption under ice ∼400 m thick. This includes the products of the largest known eruption of Icelandic subglacial rhyolite of ∼16 km3 at ca. 70 ka. We find pre-eruptive water contents in melt inclusions (H2OMI) of up to 4.8 wt%, which indicates that Icelandic rhyolite can be significantly more volatile-rich than previously thought. Our results indicate that explosive subglacial rhyolite eruptions correspond with high H2OMI, closed-system degassing, and rapid magma ascent, whereas their effusive equivalents have lower H2OMI and show open-system degassing and more sluggish ascent rates. Volatile controls on eruption style thus appear similar to those for subaerial eruptions, suggesting that ice plays a subsidiary role in influencing the behavior of subglacial rhyolitic eruptions.