We provide the dataset associated with the research article “40Ar/39Ar ages of alkali feldspar xenocrysts constrain the timing of intraplate basaltic volcanism” Matchan et al. [1]. This dataset contains major element data for 15 large anorthoclase xenocrysts (‘megacrysts’) collected from six Pleistocene eruption centres (Mount Leura, Mount Shadwell, Mount Noorat, Mount Franklin, Lake Keilambete and The Anakies (East Cone)) in the basaltic Newer Volcanic Province of south-eastern Australia. It also contains multi-collector (Argus VI) 40Ar/39Ar step-heating for 13 of these anorthoclase megacrysts. 40Ar/39Ar vacuo step-crushing experiment data is also provided for three of these megacrysts.