The stream will launch the fourth season of "American Express Unstaged," an online series that pairs notable directors with popular music acts. Vampire Weekend's concert at the Roseland Ballroom on April 28 will stream live on VEVO and YouTube.
American Express was to officially announce the live stream Tuesday.
Vampire Weekend lead singer Ezra Koenig in a statement called Buscemi "a wonderful actor, a NYC legend and a great director." Buscemi has directed four feature films, including 1996's "Trees Lounge," as well as several "Sopranos" episodes.
Vampire Weekend will release their third album, "Modern Vampires of the City," on May 14.
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