Charles Godfrey Leland's early education was in the United States, and he attended college at Princeton University. During his schooling, Leland studied languages, wrote poetry, and pursued a variety of other interests, including hermeticism, Neo-Platonism, and the writings of Rabelais and Villon. After college, Leland continued his studies in Heidelberg and Munich. In 1848 Leland attended the Sorbonne, and was involved in the Revolutions of 1848 in France, fighting at consructed barricades against the King's soldiers as a captain in the revolution.
Leland returned to America after the money given to him by his father for travel had run out, and passed the bar in Pennsylvania. Instead of practicing law, he instead began a career in journalism. As a journalist, Leland wrote for The Illustrated News in New York, the Evening Bulletin in Philadelphia and eventually took on editorial duties for Graham's Magazine, and the Philadelphia Press. In 1856 Leland married Eliza Bella "Isabel" Fisher.
Leland was also an editor for the Continental Monthly, a pro-Union Army publication. He enlisted in the Union Army in 1863, and fought at the Battle of Gettysburg. Leland coined the term "emancipation" as an alternative to "abolition" to refer to the anti-slavery position.
Leland returned to Europe in 1869, and travelled widely, eventually settling in London. In his travels, he made a study of the Gypsies, on whom he wrote more than one book. Leland began to publish a number of books on ethnography, folklore and language. His fame during his lifetime rested chiefly on his comic Hans Breitmann Ballads (1871), written in a combination of broken English and German (not to be confused, as it often has been, with Pennsylvania German). His writings on Algonquian and gypsy culture were part of the contemporary interest in pagan and Aryan traditions. He erroneously claimed to have discovered 'the fifth Celtic tongue': the form of Cant, spoken among Irish Travellers. He named it Shelta. Leland became president of the English Gypsy-Lore Society in 1888. Eleven years later Godfrey produced Aradia, or the Gospel of the Witches, reportedly containing the traditional beliefs of Italian witchcraft as conveyed to Leland in a manuscript provided by a woman named Maddalena, who Leland refers to as his "witch informant."
What is seldom mentioned in contemporary accounts of Leland's career is an aspect of his life which he viewed as of great importance, writing in his memoirs, "The story of what is to me by far the most interesting period of my life remains to be written. This embraces an account of my labour for many years in introducing Industrial Art as a branch of education in schools[.]" He was involved in a series of books on industrial arts (and crafts) including a title he co-authored in 1876 with Thomas Bolas, entitled "Pyrography or burnt-wood etching," which was revised by Frank H Ball, G J Fowler in 1900. He was, more significantly, the founder and first director of the Public Industrial Art School of Philadelphia. This school is today known as Philadelphia University of the Arts.
Leland was also an important influence on the Arts and Crafts movement. He had established a school to teach crafts to disadvantaged children in Philadelphia, which became widely known when it was praised by Oscar Wilde. Wilde later wrote to Leland he would be "recognised and honoured as one of the great pioneers and leaders of the art of the future. The Home Arts and Industries Association was founded in imitation of this initiative.
Leland's comical Hans Breitmann Ballads were his biggest success as an author during his life, but most of his books dealt with the traditions and languages of the peoples that he studied. He is best known today for Aradia, or the Gospel of the Witches, one of his three books on Italian folk traditions.