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Easy decision (thank you Google Maps): Take 74 west to 77 north to 81 north to 78 east to 278 north. No tolls, lots of mountains, and some cool small towns/cities to make a stop at (Christiansburg, Roanoake, Staunton, Harrisonburg, Winchester, Martinsburg, Hagerstown, Chambersburg, Carlisle, Harrisburg, Hamburg, Allentown, Bethlehem, Easton). Easily doable in a day, with stopping for lunch in one of those towns a recommended option. I'm also for taking 74/77 instead of US 220 at the start since although that is about 30 more miles, with gas prices low, I'd recommend since it takes the same amount of time due to the higher speed limits, less windy roads, and fewer traffic lights.
I do the Greenville, SC - South Brunswick, SC trip once a year and to Chantilly, VA twice a year. Always the I95-77-81 and then 76-287 if needed. Just one toll bridge the entire way, maybe $1-2. I-95 is crowded and the tolls are exorbitant.