The present study applied LA–ICP-MS on gem-quality emeralds from the most important sources (Afghanistan, Brazil, Colombia, Ethiopia, Madagascar, Russia, Zambia and Zimbabwe). It revealed that emeralds from Afghanistan, Brazil, Colombia and Madagascar have a relatively lower lithium content (7Li < 200 ppmw) compared to emeralds from other places (7Li > 250 ppmw). Alkali element contents as well as scandium, manganese, cobalt, nickel, zinc and gallium can further help us in obtaining accurate origin information for these emeralds. UV-Vis spectroscopy can aid in the separation of emeralds from Colombia and Afghanistan from these obtained from the other sources as the latter present pronounced iron-related bands. Intense Type-II water vibrations are observed in the infrared spectra of emeralds from Madagascar, Zambia and Zimbabwe, as well as in some samples from Afghanistan and Ethiopia, which contain higher alkali contents. A band at 2818 cm−1, supposedly attributed to chlorine, was observed only in emeralds from Colombia and Afghanistan. Samples with medium to high alkalis from Ethiopia, Madagascar, Zambia and Zimbabwe can also be separated from the others by Raman spectroscopy based on the lower or equal relative intensity of the Type I water band at around 3608 cm−1 compared to the Type II water band at around 3598 cm−1 band (with some samples from Afghanistan, Brazil and Russia presenting equal relative intensities).