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Many crystal skulls are claimed to be pre-Columbian, usually attributed to the Aztec or Maya civilizations. Mesoamerican art has numerous representations of skulls, but none of the skulls in museum collections come from documented excavations. Research carried out on several crystal skulls at the British Museum in 1967, 1996 and again in 2004 has shown that the indented lines marking the teeth (for these skulls had no separate jawbone, unlike the Mitchell-Hedges skull) were carved using jeweler's equipment (rotary tools) developed in the 19th century, making a supposed pre-Columbian origin problematic. The type of crystal was determined by examination of chlorite inclusions, and is only to be found in Madagascar and Brazil, and thus unobtainable or unknown within pre-Columbian Mesoamerica. The study concluded that the skulls were crafted in the 19th century in Germany, quite likely at workshops in the town of Idar-Oberstein renowned for crafting objects made from imported Brazilian quartz at this period in the late 19th century.

It has been established that both the British Museum and Paris's Musée de l'Homme crystal skulls were originally sold by the French antiquities dealer Eugène Boban, who was operating in Mexico City between 1860 and 1880. The British Museum crystal skull transited through New York's Tiffany's, whilst the Musée de l'Homme's crystal skull was donated by Alphonse Pinart, an ethnographer who had bought it from Boban.

An investigation carried out by the Smithsonian Institution in 1992 on a crystal skull provided by an anonymous source who claimed to have purchased it in Mexico City in 1960 and that it was of Aztec origin concluded that it, too, was made in recent years. According to the Smithsonian, Boban acquired the crystal skulls he sold from sources in Germany – findings that are in keeping with those of the British Museum.

A detailed study of the British Museum and Smithsonian crystal skulls was accepted for publication by the Journal of Archaeological Science in May 2008. Using electron microscopy and X-ray crystallography, a team of British and American researchers found that the British Museum skull was worked with a harsh abrasive substance such as corundum or diamond, and shaped using a rotary disc tool made from some suitable metal. The Smithsonian specimen had been worked with a different abrasive, namely the silicon-carbon compound carborundum which is a synthetic substance manufactured using modern industrial techniques. Since the synthesis of carborundum dates only to the 1890s and its wider availability to the 20th century, the researchers concluded "[t]he suggestion is that it was made in the 1950s or later".

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Another novel and historically unfounded speculation ties in the legend of the crystal skulls with the completion of the current Maya calendar b'ak'tun-cycle on December 21, 2012, claiming the re-uniting of the thirteen mystical skulls will forestall a catastrophe allegedly predicted or implied by the ending of this calendar. An airing of this claim appeared (among an assortment of others made) in The Mystery of the Crystal Skulls, a 2008 program produced for the Sci Fi Channel in May and shown on Discovery Channel Canada in June. Interviewees included Richard Hoagland, who attempted to link the skulls and the Maya to life on Mars, and David Hatcher Childress, proponent of lost Atlantean civilizations and anti-gravity claims.

Crystal skulls are also referenced by author Drunvalo Melchizedek in his book Serpent of Light. He writes that he came across indigenous Mayan descendants in possession of crystal skulls at ceremonies at temples in the Yucatan, which he writes contained souls of ancient Mayans who had entered the skulls to await the time when their ancient knowledge would once again be required. The book is a log of the authors experiences, which are related in a manner requiring suspension of judgment.