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In Pennsylvania, the area east of I-79, north of I-80 and west of I-81 is the most isolated. In Georgia, the area north of I-16, south of I-20 and east of U.S. 441 is the most isolated.
Location: northern Vermont - previously NM, WA, & MA
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In Massachusetts, smallest town and most isolated for sure is the town of Gosnold, year round population of 84 residents. It's a chain of small islands west of Martha's Vineyard and one island with ferry service called Cuttyhunk.
Cuttyhunk 2008 (http://www.flickr.com/photos/blackseal35/3244817369/ - broken link) by blackseal35 (http://www.flickr.com/people/blackseal35/ - broken link), on Flickr
Another tiny town is the very southwestern corner of the state bordering Conn. & NY State, little known town of Mount Washington, Mass. population 130. It has a beautiful state park with a waterfall, Bash Bish Falls.
It's not connected to anywhere by a permanent road, although there is a winter road connecting it to Manitoba. The main way to get there is by air.
There is not a single inhabited place in a 100 mile radius, and in the 100 mile radius, you're probably more likely to run into a polar bear than another person...
The closest inhabitated place is an even smaller Native reserve (Peawanuck popo 139), about 100 miles away. The closest city above 100,000 people is Thunder Bay, 500 miles away.
In South Carolina, probably would have to be somewhere along US 301 or 321. Really, anywhere south of US 278 and west of I-95 is very isolated. Closest major city is Savannah, and there's few grocery stores on the stretch.
McCormick County is the least-populated county in the state, and probably the most-isolated. 35 miles from Augusta, and closer to Athens as the crow flies than to Columbia.
Greenwood is probably the most isolated larger town. 45 miles from Greenville, 25 miles from I-26, 65 from Columbia. Small town with not that much to do except a smaller university.
Can't really go wrong anywhere in the UP of Michigan - especially the Keweenaw Peninsula. That's isolated as heck.
As reference, I live in Detroit and it takes me longer to drive to visit my relatives that live up in Hancock (part of the Keweenaw Peninsula) than it does to visit relatives on Long Island. This fact shocks a lot of people.
The UP is gorgeous...just not too convenient for Detroiters. That's why many stop at Mackinac Island and don't go much further.
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