In 1962 Hitchcock and Truffaut locked themselves away in Hollywood for a week to excavate the secrets behind the mise-en-scène in cinema. Based on the original recordings of this meeting-used to produce the mythical book Hitchcock/Truffaut-this film illustrates the greatest cinema lesson of all time and plummets us into the world of the creator of Psycho, The Birds, and Vertigo. Hitchcock's incredibly modern art is elucidated and explained by today's leading filmmakers: Martin Scorsese, David Fincher, Arnaud Desplechin, Kiyoshi Kurosawa, Wes Anderson, James Gray, Olivier Assayas, Richard Linklater, Peter Bogdanovich and Paul Schrader.

Scorsese filmed the Rolling Stones at the Beacon Theatre on October 29 and November 1, 2006, but the performance footage used in the film is all from the second show. The concert footage is preceded by a brief semi-fictionalized introduction about the preparations for the shows, and is intercut with historical news clips and archival interviews with band members. The film takes its title from the song of the same name, featured on the band's 1972 album Exile on Main St. A soundtrack album was released in April 2008

In the second episode, filmmaker Martin Scorsese examines the life of musician George Harrison, weaving together interviews, concert footage, home movies and photographs.