Nice website Alex. Enjoyed a nice rainy cold and windy OBX Saturday afternoon reading about your hike through the Henry’s from The Burr trail. And you almost got Buffaloed!
I played around with google maps out of curiosity to see what terrain in NC falls within Dalton’s 3 hour limit Since I didn’t know exactly where you are in Charlotte I made a guesstimate worst case? selection and started on the east side of town at the intersection of 485 and 27 which shows up on google as Mint Hill. Your 3 hour line ends up running from @ lake Toxaway over to Dillsboro and on to Cherokee. This means that pretty much everything south of the BRP from 215 to Newfound Gap rd. is too far. This includes the Nantahala National Forest (Standing Indian for ex.) The Bartram Trail, the AT along the Wayah-Wesser Crest and side trails, Fires Creek, the Andrews area, Snowbird, and Joyce Kilmer/Slickrock areas are out along with everything in the GSMNP south of Newfound Gap Rd. The Tennessee side of the main ridge on the East side of the park @ Cosby is probably out too though there aren’t that many trails in that quadrant.
Put another way pretty much every stretch of mountains in NC from the Blue Ridge Parkway south of Asheville over to Cherokee all the way to Virginia is within 3 hours;Â and all the rest of the NC mountains fall inside of or right on the edge of the 4 hour limit. Also that is Google’s estimated driving time. I can usually shave several minutes per hour off their estimates but there you go.
SO This leaves @ 1,524,693 options. Haha…
I was surprised to see the closest areas are The Wilson Creek/Linville Gorge/Grandfather Mt. areas, all of the Black Mt ridgeline, And the GSMNP N.E. quadrant including Cataloochee and Big Creek. I guess the latter is due to due to the fast access via I-26 and I-40. Everything else south of I-40Â to the BRP is also doable in your specified time-frame, with Panthertown for ex. just possibly squeaking in.
In most all of these locations you can devise a route going up a drainage or side ridge to a main crest then hike along the crest to the next side trail and back down. Most of these have connections of some sort.
The Grandfather section of the Pisgah National Forest including the Wilson Creek,, Grandfather Mt. and Linville Gorge areas is a maze of connected trails. Lots of really nice waterfalls. My avatar photo is a shot of my brother and oldest daughter in a beautiful carved granite pool below (and above) a stretch of cascades/ slides and waterfalls in Gragg Prong in the Wilson Creek drainage.
The Black Mt Crest and Mt. Mitchell will prepare you for pretty much any really hard trail climb almost anywhere ( except for the change in atmosphere) with several trails climbing over 4000″ in @ 6 miles.
Brad mentioned a couple of really nice routes coming out of Big Creek. You could make loops throughout the entire NC side of the northeast corner of the GSMNP including Big Creek and Cataloochee.
You also mentioned the Art Loeb Trail which follows one of the north/south oriented crests of the Great Balsam Mts. There are several side trails leading up to that crest and the Art Loeb Trail from both highway 276 to the east and highway 215 to the west.
All of these areas offer really great hiking, often with nice streams and waterfalls, stretches of large or even old growth forest (Boogerman!), and even some fairly long stretches of “bald” ridgeline with great views. Many cross some of the 54 named peaks in NC that top 6000″ out of the 56 west of the Black Hills of S. Dakota (2 of those 6,000 footers escaped NC; Le Conte when the border was drawn incorrectly ;) and Mt. Washington which is wayyyy up there in New Hampshire.
I might also recommend that if you start really getting into these trips you look up the Carolina Mt. Club’s challenge:South beyond 6000 Â https://www.carolinamountainclub.org/index.cfm/do/pages.view/id/23/page/South-Beyond-6000Â Â
By the time you finish this challenge you will very well acquainted with the mountains of North Carolina. You will also by necessity get the experience of doing a little off-trail hiking to reach some of these high points and really improve your hiking/navigation competence while visiting some spots not that far from the beaten path that don’t get too many visitors (Mark’s Knob, Potato Knob, Reinhart Knob,, oh boy lots of fun!)Â Bring a few strips of Surveyors tape to follow back to the trail and don’t be a donkey’s butt and leave them hanging!
BTW if you’re trying to hike and are concerned about snow; check out the weblog “High on LeConte”  http://www.highonleconte.com/daily-posts. If the trails are clear up there they’re pretty much clear everywhere and it’s usually fun to read anyway. There are also some other webcams like Purchase Knob. You could do a search and find at least one in almost every area.
Anyway you’ve got the potential for some serious fun ahead. Happy Trails!