Multiple competing hypotheses have been proposed to explain the source of loess dust in the Carpathian Basin yet none has been demonstrated. Here bulk and grain-size differentiated Nd and Sr isotopic and bulk and clay mineralogical compositions, together with detrital zircon ages and morphologies from loess along the Danube in the Carpathian Basin are used to demonstrate that no single method is capable of unequivocally isolating sources, yet combined, they allow for discriminating likely provenance. Zircon ages indicate multiple sources for Carpathian Basin loess, restricting the use of bulk or grain-size differentiation methods. Ambiguities are further highlighted by the fact that the Sr–Nd isotopic composition of Greenland dust is very similar to Carpathian loess. This match demonstrates that such methods are not always capable of unequivocally excluding unlikely potential source areas and implies that current hypotheses regarding the origin of Greenland dust require further evaluation. Sr isotopes are also limited by high dolomite contents of loess, while palygorskite is of questionable utility as a Saharan dust indicator due to its rapid weathering under typical Carpathian climates. In terms of specific Carpathian loess sources, alluvial fans of the Danube River likely contribute, but detrital zircon ages and morphologies suggest that a proportion directly originates from eroded uplands and local rocks throughout the basin, while detrital dolomite implies local, primary sources such as the Transdanubian Range. An upper limit of 5–10% is placed on the North African contribution to fine dust in loess of the mid-Carpathian Basin based on mineralogy and grain size. Overall, results suggest that the single grain (zircon) approach is likely the most diagnostic method to identify sources in loess studies, although to solve complex provenance issues, simultaneous consideration of the isotopic characteristics of more than one heavy (or light) mineral is required.