Look up Jim Casada, he is THE author for smokies fishing.
I have a buddy who fishes tenkara and runs a fly shop/guide service out of Cherokee. Justin Hunt, Rivers Edge Outfitters. He’s a great dude, and he fishes a crap ton in and very near the park.
When are you looking to go? That’s only 4-5hrs away from me, depending on traffic, maybe I could meet up with you?
EDIT- I see now you’re looking at September. Whoa that’s a long way’s out, plenty of time to put together a solid plan.
Smokemont is the nicest frontcountry campground on the NC side, and the only one that you can make reservations for individual sites at (not just group). Actually I think you can reserve in Cataloochee too, and it’s supposed to be really nice. Will you be doing front or backcountry? If you want to see more than just one small part of the park, you will want to stay somewhere on or very close to 441, so that you can cross over to the other side.
September can go either way- if it’s a rough summer like we had in 2016, the fishing may be terrible, with low water levels. We’re having a great winter with lots of snow up that way, so hopefully that continues and this summer is a good one. October (late) is when the fall colors start, and that’s prob the busiest time of the year for the park and that region.
Balsam Mountain campground is one I’ve been wanting to check out- it’s the highest elev frontcountry site w/ bathroom in the park.
Bryson City is a great little city with a couple nice places to eat, two breweries (Mountain Layers is awesome!), Great Smoky (no “e”) Mountain Railroad, and a nice fly shop. It’s right outside the Deep Creek portion of the park, which is cut off from the rest of GSMNP.
Cherokee is suuuuuuuuuuper touristy, you should avoid it other than passing through, or going to Rivers Edge Outfitters (my preferred fly shop on NC side of the park). Cherokee is at the Oconaluftee Visitor Center entrance to the park, where Smokemont is, and 441 which takes you over to TN.
Asheville is awesome, about an hour up the road. LOADS of good beer and food. Maggie Valley is just outside Cataloochee, and somewhat isolated.
I mostly have experience on the NC side, and haven’t been able to do nearly as much fishing in the park as I’d like to, but I have gathered a LOT of info over the years of research lol.
If you are staying in Cherokee/Bryson City/Smokemont, I would HIGHLY HIGHLY HIGHLY suggest fishing the Straight Fork of the Raven Fork… Look it up. It’s a branch of the Raven Fork (river?) on the SE side of the park, comes out of one of the most remote sections of the park and flows into Cherokee. The Tribe stocks it with big dumb pellet heads in their section, but a very short distance into the park, and it’s all wild fish, all beautiful, and a great place to try for a slam. You drive up the dirt rd following the stream, and it’s one of the least-visited sections of the park, mostly just anglers go out there, since there is only fishing and hiking, and it’s serious hiking at that.