The brochures can point you in the right direction. If you're going to be in the Gatlinburg area, and up to a good hike, the Abrahms Falls trail should have some good fishing at the end, in the falls area. It pools up nicely there, and last time I was there (be it around 10 years ago) there were a ton of good sized bass in the pool.
Shoot, I used to catch trout in the stream in downtown Gatlinburg.
The Little Pigeon River that runs through Pigeon Forge, etc, is supposed to be a good smallmouth river, from what I've heard.
If I remember correctly, all lures must have barbless hooks (maybe single barbless?) on them in the national park waters.