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I passed through on the AT a couple years ago. Charlie's Bunyon is cool, and supposedly a less-seen part of the park. If you're looking for a tough hike, I've heard Shuckstack is pretty tough, though the route up on the AT is not very difficult. Highest point in the park is Clingman's Dome, but I didn't think it was that great. Plus it's accessible by road, so there are a lot of tourists.