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I would head north out of Greenville on 276 and follow it to 64 then all the way to Franklin, NC then north on 28 to 129 (The Dragon). Then work your way over in TN to Arkansas (there is nothing really good for driving in Northern MS). In AR you can go North to Harrison and Eureka Springs or go South through Hot Springs and on to Mena and the Talihina Scenic Byway and on into OK. Both are good routes.
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