The High is dedicated to supporting and collecting works by Southern artists and is distinguished as the first general museum in North America to have a full-time curator devoted to folk and self-taught art.

The nucleus of the folk art collection is the T. Marshall Hahn Collection, donated in 1996, and Judith Alexander's gift of 130 works by Atlanta artist Nellie Mae Rowe.

Other artists the High has collected in depth in this field include the Reverend Howard Finster, Bill Traylor, Thornton Dial, Ulysses Davis, Sam Doyle, William Hawkins, Mattie Lou O'Kelley, and Louis Monza. The collection of almost 800 objects also boasts superb examples by renowned artists from beyond the South, such as Henry Darger, Martín Ramírez, and Joseph Yoakum.