After making a remix for a charity record, Simon Posford (Shpongle, Hallucinogen) and Benji Vaughan (Prometheus) formed the band.
The album A Flock of Bleeps released on Twisted Records became a cult classic in the underground electronica scene[citation needed] and included such tracks as "Crumblenaut" and "Finger".
2009 saw Younger Brother produce "Phoenix in Dynamite Sky" for British cult film Heartless, directed by Philip Ridley.
Their third album Vaccine, recorded with its U.S. band lineup (Marc Brownstein of The Disco Biscuits, Joe Russo of Benevento/Russo Duo and Furthur & Tom Hamilton of Brothers Past), became available on 4 April 2011.
In 2014, the band developed an app for mobile devices and released an alternate album of remixes titled Vaccine Electronic as a free stream for users who installed it.