The band gained some notoriety in the early 2000s. Although their mainstream success was initially limited, their profile soon grew, culminating in a #2 single and #1 album in the UK Charts. In December 2004, their self-titled second album was voted the second best album of the year by NME magazine. Both of their full-length LPs were produced by Mick Jones, of the British punk band The Clash.

In spite of their critical success, the band's music was often eclipsed by its internal conflicts, stemming from Doherty's addictions to crack cocaine and heroin, which eventually led to the breakup of the band. Doherty has since stated that the breakup of the band was due to relationship difficulties between Barât and himself that were not related to his drug addictions. The members of The Libertines went on to form new bands with varying degrees of commercial and critical success.