Completed in 1851 for use as a library, this National Historic Landmark was originally named Smith Hall in honor of Benjamin Smith. Smith, a special aide to George Washington during the American Revolution and state senator and governor of North Carolina, donated land to the University.

Proceeds from the sale of the land became the first major benefaction to Carolina. Architect Alexander Jackson Davis made a noticeable change in the usual adornment of Corinthian capitals across the portico. Instead of acanthus leaves, Davis used wheat and Indian corn in keeping with the growing allegiance to the young nation called America.

Smith Hall became the University's library, although use was suspended when Federal soldiers stabled their horses in Smith Hall during part of the Civil War. After a two-year span in which the books were moved to South Building, Smith Hall again became the main library in 1870. Despite disuse when the University closed between 1871 and 1875, the collection grew to nearly 40,000 volumes by 1900. When the library moved to a new building in 1907, the School of Law occupied Smith Hall until 1923. In 1925, the structure was renovated for use by the Carolina Playmakers.

Today, the building hosts student drama productions, lectures, and concerts and events sponsored by academic departments.