First of all, once you get a mile from a trailhead, you loose most of the dayhikers, so don't worry about that. Cataloochee is very popular with dayhikers and car campers and horse riders, but it is for a reason, a very beautiful and historic area.
OK, from the Deep Creek area I haven't hiked that loop, but I have done a little in the area. Start at the end of Lakeview Drive (Road to Nowhere) and hike to 70 for your first day, then the Jonas Creek Trail (wet feet) up to the AT and across to Clingmans Dome (amazing views, but you will see tourists, it is worth it), then down to Andrews Bald followed by a slight backtrack to Forney Creek trail and site 68 for the second day. Then down Forney Creek and across Springhouse Branch to Noland Branch and site 64 for the third day, then down Noland Creek to the road and ~.5 mile road walk to the car.
This loop will get you some ridge hiking and great views, some classic creeks, and other than the Clingmans Dome and Andrews Bald stretch, you won't see a lot of people (only backpackers).
I haven't stayed at 68, but it is very close to some Cascades that look pretty cool. Every trip that I have tried to do this loop, something has gone wrong, but I'm usually in the park in the winter time. I also haven't hiked along Noland Creek, but it is a classic Smokies creek trail and that means nice hiking.
Next to Site 70
View from the tower at Clingmans Dome
View from Andrews Bald