This was my master plan when I was out there last year, even though we cut it short... then did the Blue Ridge Parkway the next day. The drive north of Cherokee should be pretty fun, but for whatever reason there was a decent amount of traffic on it at the time. Tail of the Dragon was a lot of fun, but would have been even better on a bike.... Cherohala Skyway was okay, I wouldn't do it again. Blue Ridge Parkway wasn't as fun of a drive overall, but was nice and scenic.
Didn't do a lot outside of driving, but did go to Grandfather Mountain, which has a suspension bridge you can walk across at the top.