The story of these little crystals begins over 500 million years ago as sedimentary rocks were deposited along the coastline of a continent we call Laurentia – predecessor to modern day North America. Those sediments were deposited in a passive margin – an area with no active continental boundary, formed when the supercontinent Rodinia rifted apart to form a new ocean. 300 million years ago or so, that ocean closed as what is today Northwest Africa collided with eastern Laurentia, uplifting a huge mountain range. The sediments that were originally deposited off the coast of Laurentia were trapped in this mountain range. They were shoved deep into the Earth’s crust and heated, so much so that the minerals in the rock changed – making the sediments into a metamorphic rock.
One of the metamorphic minerals produced under these conditions is the mineral staurolite. Staurolite has a neat property to its structure called twinning – the layers of atoms that make up the mineral will sometimes shift along a plane or surface inside the mineral, and they do so in specific patterns. Staurolite twins by creating either 60 or 90 degree angles inside the crystal – basically forming two crystals that interlock, into a cross shape.
These staurolite crystals grew during the metamorphic event caused as the Appalachians formed. Eventually Africa and North America separated and these rocks were pulled back to the surface by new faults and erosion of the mountains above. As they cooled off, the staurolite converted to sericite, a lower-temperature mineral, without changing shape – a process called pseudomorphing (one mineral in the shape of another).
Given the religious significance of the cross shape, and the fact that they’re just neat in the first place, it’s not hard to see why these stones became collectable. Even imperfect stones can be used – the sericite is soft enough to be easily cleaned and polished and shaped into perfect crosses. In fact, I even found a literature reference from 1934 of one of them being polished into a Swastika. These stones are picked out of Fairy Stone State Park in Virginia – they are free to collect as long as you use only your hands and pay admission/parking fees in the park.