Cave deposits of infill sediments and associated vertebrate fossils provide a valuable source of information on terrestrial palaeoenvironments, climatic conditions and palaeocommunities. In the deposits of the Naracoorte Caves World Heritage Area, such records span the last 500 ka and are renowned for their rich, diverse vertebrate assemblages. Previous research into the Grant Hall deposit of Victoria Fossil Cave suggested that it may preserve the only peak last interglacial (ca. 125 ka) faunal community within the World Heritage Area. The current work tested this existing model for the age of faunal remains from Grant Hall using multiple techniques. Physical and geochemical properties of the visually homogeneous sediments were analysed at regular intervals through the sequence to establish meaningful stratigraphic divisions and sediment provenance. Optically stimulated luminescence dating of individual quartz grains indicates that sediments accumulated in Grant Hall from 93 ± 8 to 70 ± 5 ka. Minimum ages provided by U/Th dating of fossil teeth (72.3 ± 2.2 to 38.2 ± 0.8 ka) are consistent with the luminescence chronology, and show that the deposit represents a more recent faunal accumulation than previously modelled for the site. U/Th ages on calcite straws within the deposit are significantly older than the sediments and fossil teeth (>500 to 186.4 ± 1 ka). As such they provide no further constraint on the chronology of the deposit but do indicate that speleothem deposition was active over much of the Middle Pleistocene. Sedimentary analyses resulted in the identification of five depositional units, contrasting with previous divisions which were based only on visual observation of the sedimentary sequence. Sediments within each unit are broadly classified as sandy silts with soil structures and may be indirectly derived from the lunettes of nearby Bool Lagoon, although their ultimate provenance is unknown. As a result of this work, palaeoenvironmental reconstruction based on fossil remains in the deposit may be more accurately related to prevailing climatic and environmental conditions at the time of accumulation. It also contributes to an understanding of the temporal occurrence of regional vertebrate faunas through the Late Pleistocene, reinforcing the value of developing stratigraphically constrained chronologies for cave deposits based on multiple techniques.