Smokehole Road is definitely a must do.
If you decide to venture into VA, a couple of my favorites in that part of the world... in no special order... Rte 250... the piece of 250 in VA is my favorite but it's a good road all the way into WV. Look up the piece between West Augusta, VA & Monterey, VA... but like I said, it's good all the way into WV. Also high on my list in VA is Rte 56. The piece from Roseland, VA to Vesuvius, VA is awesome! Rte 60 has a good piece of road running up & over the Blue Ridge Parkway.
If you decide you'd like to try Rte 250 into WV, here's a hint... take 250 into Durbin & make a left onto Back Mountain Rd. BMR isn't a beat feet kinda road. It's kinda pig trailish a little but not really in a bad way... views are awesome! Also, BMR will dump you out in Cass, WV which houses
Cass Scenic Railroad. Cass Railroad is something you may be interested in seeing.
From there I'd go 66 out to 219... or catch the other end of BMR off of 66 which will dump you out near Marlinton, WV/Rte 219. A good place to stay... Old Clark Inn. Old Clark is in Marlinton.
There are plenty of play areas on 219. Look @ Google Maps. It's also a direct shot to Lewisburg if you're interested in going that far south.