Born and raised in Fitzgerald, Georgia, Mayes attended Randolph-Macon Woman's College in Lynchburg, Virginia, and obtained her BA from the University of Florida. In 1975 she earned her MA from San Francisco State University, where she eventually became Professor of Creative Writing, director of The Poetry Center, and chair of the Department of Creative Writing.
Mayes has published several works of poetry: Climbing Aconcagua (1977), Sunday in Another Country (1977), After Such Pleasures (1979), The Arts of Fire (1982), Hours (1984), and Ex Voto (1995). In 1996 she published the book Under the Tuscan Sun: At Home in Italy, which was on the New York Times Best Seller list for over two years. The book is a memoir of Mayes buying, renovating, and living in an abandoned villa in rural Cortona in Tuscany, a region of Italy. A film loosely based on the book, Under the Tuscan Sun. was released in 2003, adapted by director Audrey Wells. In 1999, Bella Tuscany: The Sweet Life in Italy was published, and in 2000, In Tuscany. Mayes's first novel, Swan, was published in 2002. The book Bringing Tuscany Home was published in 2004, a collaborative effort of Mayes and her husband Edward Kleinschmidt Mayes with photographer Steven Rothfeld. Another memoir, Every Day in Tuscany, was released in March 2010.
Also a food-and-travel writer, Mayes is the editor of The Best American Travel Writing 2002 and the author of A Year in the World: Journeys of A Passionate Traveller (2006), narratives of her and her husband's travels in Greece, Turkey, Spain, Morocco and other countries.

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