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Portable X-ray fluorescence (pXRF) spectrometry was used to obtain source determinations for 11 obsidian artefacts from five archaeological sites in Bulgaria. The results show that all the archaeological specimens can be linked to obsidian sources in the Carpathian Mountains in the border region between Hungary and Slovakia. Obsidian from the C2E source in Hungary occurred in very early Neolithic contexts at Dzhulyunitsa, while the majority of samples from later contexts at Ohoden, Dzherman and Varna came mainly from the Slovakian (C1) source. The data hint at a shift from the use of C2 obsidian in the Neolithic before 5900 cal BC, to a preference for C1 obsidian in later periods – however, more finds and better contextual and chronological data are required to verify this trend.