The Carlos Museum's collection of African art offers valuable insight into African artistic expressions in the variety of their forms, functions, and cultures of origin. A majority of the objects come from the collection of William S. Arnett acquired by the museum in 1994. Arnett collected masks and carved figures from West and Central Africa, particularly the numerous cultures of Nigeria, Benin (formerly Dahomey), the Cameroon Grassfields, and the Democratic Republic of the Congo. Since 2003 the African collection has grown through select acquisitions and gifts to represent objects from East and Southern Africa, including textiles, ceramics, and jewelry.

Made from a variety of indigenous and imported materials, the objects in this collection bear evidence of uses in a variety of contexts, both religious and secular. There are figures from personal or family shrines, such as the Fon Asen Altar, complemented by those used in community shrines, such as the Urhobo Figure and the Ethiopian Processional Cross. There are examples of secular art, generally made to be seen in public to communicate ideas about status, wealth and identity, like the exquisite Beaded Bowl Figure from the Kom kingdom of the Cameroon Grassfields, used by royalty to hold kola nuts for their guests, and the Ndebele woman’s Beaded Cape from South Africa. The collection also includes a wide variety of masks like the Igbo Maiden Spirit Mask, danced in masquerades that carry religious and cultural significance for participants, including the audience. All these works demonstrate important aspects of the worldviews and aesthetic values of their cultures of origin.