The song was an early favorite for the band and is rumored to have led to their meeting with future manager Andy Warhol. In late 1965 the Velvets were booked to play at the Café Bizarre in Greenwich Village, however the gigs did not attract many people (according to Cale the club was made up almost exclusively of drunks) and the club's owner insisted on them fulfilling every minute of their booked time, with the final straw being a long gig on Christmas Eve. The band began playing long improvised versions of "Black Angel's Death Song" to the point where they were threatened with the sack if they performed it one more time. On 11 November 1965, The Velvets retorted with an even longer grand finale of the song. On their way out they were approached by a member of the audience, Andy Warhol, who within five months was producing their debut album.
Recorded April 1966, at Scepter Studios in Manhattan, the music is dominated by the piercing sound of John Cale's electric viola, creating dissonance throughout the song. Also throughout the song are loud bursts of audio feedback, primarily from Cale hissing into the microphone. The guitars in the song are downtuned a whole step (as is common with a handful of other songs on The Velvet Underground & Nico).