Sulphate records from Greenland ice-cores indicate that Marine Isotope Stages 4 and 5 were characterised by a higher incidence of large volcanic eruptions than other periods during the last glacial period, however, few investigations have focused on tephra deposits associated with these volcanic eruptions and the nature and origin of the events. Here we present a detailed tephrochronological framework of the products of 15 volcanic events spanning this interval; the majority of which have been preserved as cryptotephra horizons within the Greenland records. The major element compositions of individual glass shards within these horizons indicate that 13 of the eruptions originated from Iceland and 6 of these events can be correlated to the specific volcanic systems of Katla, Grímsvötn, Grímsvötn-Kverkfjöll and either Reykjanes or Veidivötn-Bárdarbunga. For the remaining Icelandic horizons a source from either the rift zone or a flank zone can be suggested based on rock suite affinities. Two horizons have been correlated to a source from the Jan Mayen volcanic system which represents the first discovery of material from this system within any Greenland ice-cores. The robust geochemical characterisations, independent ages for these horizons (derived from the GICC05 ice-core chronology) and stratigraphic positions relative to the Dansgaard-Oeschger climate events recorded in the Greenland ice-cores represent a critical framework that provides new information on the frequency and nature of volcanic events occurring in the North Atlantic region during MIS 4 and 5. This framework can now be utilised in the assessment of the differential timing and rate of response to the millennial-scale climatic events that characterised this period, through the use of the tephra horizons as time-synchronous tie-lines to other palaeoclimatic sequences.