Yes, go further north on 19 and look for a sign pointing to Helton Falls not too far on the other side of the Appalacian Trail crossing. Its bigger and prettier than De Soto. Also you can double back and take 60 west and go to Dockery Lake. It's the feeder to Waters Creek and has a sliding type waterfall downstream from the dam, but its very difficult to get a good view of it. You can continue west and take the road to the fish hatchery on Little Rock Creek and possibley find the waterfall there. The parking spot is where the road hairpins right at a bridge over the creek, you follow the left side of the gorge to the falls. Theres a bunch of other places but I'd need to get my waterfall book out and would take way too long. I think Unicoi is not very far from there either.
Just be sure you don't turn around too soon to see the second falls. Theres good cascades all along the creek, some accesible. Hope your vehicle has some ground clearance, theres a stream crossing way past the second falls and nice scenery beyond.