Dear Catastrophe Waitress, The Life Pursuit and hiatus (2003–2010)
The band left Jeepster in 2002, signing a four-album deal with Rough Trade Records. Their first album for Rough Trade, Dear Catastrophe Waitress, was released in 2003 and was produced by Trevor Horn. The album showed a markedly more "produced" sound compared to their first four LPs, as the band was making a concerted effort to produce more "radio-friendly" music. At this point, the band began to engage more with the press and started appearing in publicity shots. The album was warmly received and is credited with restoring the band's "indie cred". The album also marked the return of Murdoch as the group's primary songwriter, following the poorly received Fold Your Hands Child, You Walk Like a Peasant and Storytelling, both of which were more collaborative than the band's early work. A documentary DVD, Fans Only, was released by Jeepster in October 2003, featuring promotional videos, live clips and unreleased footage. A single from the album, "Step into My Office, Baby" followed in November 2003; it would be their first single to be taken from an album, and included a track recorded with Divine Comedy producer Darren Allison entitled Love on the March.
The Thin Lizzy-inspired "I'm a Cuckoo" was the second single from the album. It achieved their highest chart position yet, reaching No. 14 in the UK. The Books EP followed, a double A-side single led by "Wrapped Up in Books" from Dear Catastrophe Waitress and the new "Your Cover's Blown". This EP became the band's third top 20 UK release, and the band was nominated for both the Mercury Music Prize and an Ivor Novello Award. In January 2005, B&S was voted Scotland's greatest band in a poll by The List, beating Simple Minds, Idlewild, Travis, Franz Ferdinand, and the Proclaimers, among others.
In April 2005, members of the band visited Israel and the Palestinian territories with the UK charity War on Want; the group subsequently recorded a song inspired by the trip titled "The Eighth Station of the Cross Kebab House", which would first appear on the digital-download version of the charity album Help!: A Day in the Life and would later have a physical release as a B-side on 2006's "Funny Little Frog" single. Push Barman to Open Old Wounds, a compilation of the Jeepster singles and EPs, was released in May 2005 while the band were recording their seventh album in California. The result of the sessions was The Life Pursuit, produced by Tony Hoffer. The album, originally intended to be a double album, became the band's highest-charting album upon its release in February 2006, peaking at No. 8 in the UK and No. 65 on the US Billboard 200. "Funny Little Frog", which preceded it, also proved to be their highest-charting single, debuting at No. 13.
On 6 July 2006, the band played a historic show with the Los Angeles Philharmonic at the Hollywood Bowl. The opening act at the 18,000 seat sell-out concert was the Shins. The members of the band see this as a landmark event, with Stevie Jackson saying, "This is the biggest thrill of my entire life". In October 2006, members of the band helped put together a CD collection of new songs for children titled Colours Are Brighter, with the involvement of major bands such as Franz Ferdinand and the Flaming Lips.
On 18 November 2008 the band released The BBC Sessions, which features songs from the period of 1996–2001 (including the last recordings featuring Isobel Campbell before she left the band), along with a second disc featuring a recording of a live performance in Belfast from Christmas 2001.