Morgan Joyce Varn, 24, was arrested after she invited a man to her home in order to rob him at gunpoint, says Lancaster County Sheriff's Office.
She has been charged with armed robbery, kidnapping, and malicious injury to personal property.
It is unclear whether she has had a procedure to tattoo her eyeballs, or if she was wearing special contact lenses.
One news website in Las Vegas posted the image to its Facebook account with the caption: "Here's a Mugshot to Haunt Your Nightmares."
"Exorcist needed ASAP," read one online comment.
Ms Varn and two others were arrested last Monday night in the community of Indian Land after an hours-long standoff with armed police.
A police mugshot of a South Carolina woman is drawing attention due to her striking black eyeballs.