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The following explanation is from "The Book of Totally Useless Information" by Don Voorhees:

Why is North Carolina Called te "Tarheel State"?

One product North Carolina was famous for throughout its history was tar.

During the Civil War many heated battles were fought in North Carolina and the local regiments were dedicated rebel soldiers. During one particularly fierce battle, several other Confederate troops began to retreat, leaving the North Carolina regiments to fight on alone. The North Carolinians became incensed at the retreating "cowards."

Supposedly, the North Carolinians yelled that they would put tar on the heels of the retreating rebels so they would stick better during the next battle.

Other versions of the story, not popular in North Carolina, have it that a brigade of North Carolina soldiers retreated from their position during the battle and were chided by a Mississippi brigade to tar their heels before the next battle.

Regardless of the origin, North Carolina is now proudly known as the Tarheel State.