The name Mephistopheles is associated with the Faust legend of an ambitious scholar, based on the historical Johann Georg Faust. In the legend, Faust makes a deal with the Devil at the price of his soul, Mephistopheles acting as the Devil's agent.

The name appears in the late-16th-century Faust chapbooks- stories concerning the life of Johann Georg Faust, written by an anonymous German author.

In the 1725 version, which Goethe read, Mephostophiles is a devil in the form of a greyfriar summoned by Faust in a wood outside Wittenberg.

From the chapbooks, the name entered Faustian literature. Many authors have used it, from Goethe to Christopher Marlowe. In the 1616 edition of Marlowe's The Tragical History of Doctor Faustus, Mephostophiles became Mephistophilis.

Mephistopheles in later treatments of the Faust material frequently figures as a title character: in Meyer Lutz' Mephistopheles, or Faust and Marguerite (1855), Arrigo Boito's Mefistofele (1868), Klaus Mann's Mephisto, and Franz Liszt's Mephisto Waltzes. There are also many parallels with the character of Mephistopheles and the character Lord Henry Wotton in The Picture of Dorian Gray by Oscar Wilde.