The 64-year-old actor will feature in the latest film in the Cities of Love series, according to The Hollywood Reporter.
Rourke will play a divorced man whose intimacy with a young female stranger causes him to question the identity of his estranged daughter.
The "Iron Man 2" star will star in the Til Schweiger- directed segment.
The ensemble cast also boasts big names such as Diego Luna, Orlando Bloom, Sophie Turner, Jack Huston and Jared Leto, with actors Renee Zellweger and Patrick Dempsey also making their directorial debuts in the film.
The franchise has also included stops in Paris ("Paris je t'aime") 2006 and New York City ("New York, I Love You") in 2008.