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Ajo (pronounced ah-ho) is the Spanish word for garlic. The Spanish may have named the place using the familiar word in place of the similar-sounding O'odham word for paint (oʼoho). The Tohono O'odham people obtained red paint pigments from the area.

Native Americans, Spaniards and Americans have all extracted mineral wealth from Ajo's abundant ore deposits. In the early nineteenth century, there was a Spanish mine nicknamed "Old Bat Hole". It was later abandoned due to Indian raids. The first Anglo in Ajo, Tom Childs, on the way to the silver mines near Magdalena de Kino, Sonora, arrived in 1847 and found the deserted mine complete with a 60-foot shaft, mesquite ladders, and rawhide buckets. High-grade native copper made Ajo the first copper mine in Arizona. Soon the Arizona Mining & Trading company, formed by Peter M. Brady, a friend of Childs, worked the rich surface ores, shipping loads around Cape Horn for smelting in Swansea, Wales, in the mid 1880s. The mine closed when a ship sank off the coast of Patagonia. Long supply lines and the lack of water discouraged large mining companies

With the advent of new recovery methods for low-grade ore, Ajo boomed. In 1911, Col. John Campbell Greenway, a Rough Rider and star Yale athlete, bought the New Cornelia mine from John Boddie. He became general manager of the Calumet and the Arizona mining company and expanded it on a grand scale. In 1921, Phelps Dodge, the nation's largest copper company, bought New Cornelia and the mine became the New Cornelia Branch of Phelps Dodge, managed by Michael Curley. For several decades more than 1,000 men worked for Phelps Dodge in the open pit mine. The mine closed in 1985, following a bitter strike and a depressed copper market.