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Originally released in March 1967 and written by Syd Barrett. The song's title character is a transvestite whose primary pastime is stealing women's clothes and undergarments from washing lines. According to Roger Waters, "Arnold Layne" was actually based on a real person: "Both my mother and Syd's mother had students as lodgers because there was a girls' college up the road so there were constantly great lines of bras and knickers on our washing lines and 'Arnold' or whoever he was, had bits off our washing lines."

"Arnold Layne" regularly ran for ten to fifteen minutes in concert (with extended instrumental passages), but the band knew that it had to be shortened for use as a single. It was a complex recording involving some tricky editing, recalling that the middle instrumental section with Richard Wright's organ solo was recorded as an edit piece and spliced into the song for the final mix. Both "Arnold Layne" and "Candy and a Currant Bun" were mixed into mono for the single. Neither have ever been given a stereo mix, although the four-track master tapes still exist in the EMI tape archive.

Studio version