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The music of FLCL was largely written and performed by The Pillows, which has generated mass success and appreciation since the series' release abroad. The ending theme is The Pillows' "Ride on Shooting Star". The remaining music was written by Shinkichi Mitsumune. Two soundtrack CDs — Addict and King of Pirates — and a one-CD "best-of" compilation (FLCL No. 3) were released in Japan and later in America.

Six pieces of theme music are used for the episodes; five opening themes and one closing theme. All the theme songs are by the Japanese rock band The Pillows, whose music is featured in the series. The opening themes are: "One Life," used in episode one; "Instant Music" in episodes two and three; "Happy Bivouac" for episode four; "Runners High", utilized in episode five, and "Carnival" in episode six. The closing theme is "Ride on Shooting Star," used for all of the episodes. Geneon Entertainment has released the three original soundtracks encompassing the aforementioned songs, with Addict being released on January 20, 2004, King of Pirates released on September 7, 2004, and FLCL No. 3 released on June 7, 2005.

A fourth album, FooL on CooL generation, was released by The Pillows that covers songs used in both FLCL Progressive and FLCL Alternative. Released on September 5, 2018 in Japan, the album includes exclusive FLCL cover art referencing central character Haruko Haruhara and the tracks within in English and French.

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