After the success of their first single "Sound of the Underground", the newly formed group took several months to record their debut album. Also entitled Sound of the Underground, this was released on 26 May 2003 and entered the charts at number two. One of the tracks, "Girls Allowed", was written for the group by ex-Westlifestar Bryan McFadden, while "Some Kind of Miracle" was co-written by former B*Witched member Edele Lynch. The group's second single, the number two hit "No Good Advice", was also released in May 2003, and the third single, "Life Got Cold", charted at number three in August 2003.

In November 2003, the group released "Jump"—a cover of the Pointer Sisters' 1980s dance hit. The song featured on the soundtrack to the 2003 film Love Actually, and entered the chart at number two. The album went platinum after a re-issue was released on 1 December 2003. The new version of Sound of the Underground featured a new album cover and the replacement of three original songs with "Jump" (which was not included on the original version), "You Freak Me Out" (which appeared on the soundtrack of Freaky Friday) and "Girls on Film" (a cover of a Duran Duran song originally a B-side to "Life Got Cold"). "You Freak Me Out" was included on release schedules and was performed on CD:UK in early 2004, with presenter Cat Deeley stating that it would be their next single. However, the plans for this release were scrapped as work began on a second album. Sound of the Underground stayed on the top 75 chart for 20 non-consecutive weeks, over a period of more than three years (it re-entered in December 2006).

After a brief break, the group returned in June 2004 to promote their new single "The Show", the first release from their second album. It had an unusual structure for a pop song, consisting of a number of interchanged sections rather than the more typical verse-chorus form. This single showed off a new look for the group and was backed by a pre-release promotional campaign featuring five empty chairs bearing the members' names. This built up excitement over the new look, and the image later featured on the single cover with the members in their seats. When released, the single entered the charts at number two. The follow-up release, "Love Machine", also peaked at number two in September 2004. "Love Machine" was nominated for ITV's The Record of the Year and finished in sixth place. Their seventh single, a cover of The Pretenders' hit "I'll Stand by You", reached the number one position on the UK singles chart in November 2004, and stayed there for two weeks. This was 2004's single for the Children In Need appeal with its proceeds going towards the charity.

What Will the Neighbours Say? was released on 29 November 2004 and entered the album charts at number six. The album featured the production and song writing skills of Xenomania. The album's immediate success led to the girls announcing their first What Will the Neighbours Say? Live tour, which took place in May 2005. What Will the Neighbours Say? received excellent reviews; most critics deemed it an improvement on their debut release. The final single to be taken from this album was "Wake Me Up", released in February 2005. It charted at number four—their first to miss the top three, but their eighth top-five single. In early 2005, the group won Glamour Magazine's "Band of the Year" award, and were also nominated for a BRIT Award for Best Pop Act.

After a short break following their first tour, the group began work on their third studio album, Chemistry. The first single from the album, "Long Hot Summer", was released in August 2005 and charted at number seven, ending their consecutive top five run but continuing their unbroken run of top ten singles. The single that launched their third album was "Biology" which peaked at number four. Chemistry was released on 5 December 2005. The album peaked on the charts at number eleven, their lowest so far, despite overwhelming critical acclaim; it has also gone platinum.

Their cover of Dee C. Lee's "See the Day", released in the Christmas week of 2005, charted at number nine. "See the Day" became Girls Aloud's biggest hit in terms of radio airplay since "Sound of the Underground", peaking at number six due to its success on stations such as BBC Radio 2. Girls Aloud released their debut DVD Girls on Film in June 2005, featuring their first eight music videos and television performances. It peaked at number five on the DVD Music chart. This was followed by the What Will the Neighbours Say? Live DVD in November 2005, which reached number six. The group travelled to Australia and New Zealand in February 2006 to release the single "Biology" and the album Chemistry. Arriving on 23 February, the group undertook a one-week promotional tour, during which they appeared on many TV shows. "Biology" peaked at number twenty-six in the Australian singles chart, failing to break the group in the Australian market.

"Whole Lotta History" was the fourth and final single to be taken from Chemistry. Released in March 2006, it reached number six, the week's highest new entry. The single was accompanied by a video filmed in Paris, their first outside the UK. In May 2006 the group embarked on their second UK tour (and first arena tour), Chemistry Tour. During the tour, the girls performed at ten large arenas in the UK, playing to over 100,000 people in total. The tour received rave reviews, with the majority of tabloids awarding 4/5 marks. In the same month, Girls Aloud were moved to Fascination Records, a sub-label of Polydor Records; all future Girls Aloud releases will be published by Fascination Records. Girls Aloud also won the HeartAward for the single "See the Day" at the O2 Silver Clef Lunch.

In September 2006, the official Girls Aloud web site confirmed the release of The Sound of Girls Aloud, a compilation that contains Girls Aloud's singles and some new and previously unreleased material. The album was released on 30 October 2006, and debuted at number one on the UK album chart. The album was also released on a limited edition double CD format containing live tracks such as "I Predict a Riot" and previously unavailable tracks such as "Singapore" and "Hanging on the Telephone", a cover of the Blondie single; this has now become a highly priced collectors' item.

Girls Aloud collaborated with the Sugababeson their fifteenth single, a cover of the song "Walk This Way" by Aerosmith. The track was released in March 2007 as the official single for Comic Relief, as "Sugababesvs. Girls Aloud". It became the group's third British number-one, and their fifteenth consecutive top-ten single. In May 2007, Girls Aloud went on their third tour, The Sound of Girls Aloud: The Greatest Hits Tour. During the tour, the group appeared at 15 arenas across the UK and Ireland. The supporting acts for this tour were Misha Williams, Natalia and Rogue Traders.

The song "Sexy! No No No...", the first single from Girls Aloud's fourth studio album, was released in August 2007 and reached number five on the UK Singles Chart. The album, Tangled Up, was released on 19 November 2007, debuting on the UK Albums Chart at number four. Their seventeenth single, "Call the Shots", was released in the UK one week later, and rose to number three to give the band their tenth top three single. It spent nineteen weeks in the top fifty.

Girls Aloud received their second BRIT Award nomination in 2008, nominated for the Best British Group award. Tangled Up was also certified Platinum in January. The third and final single from Tangled Up was "Can't Speak French". The single was released in March 2008, with a French version and "Hoxton Heroes", a satirical track aimed towards indie bands, as B-sides. It entered the official UK charts at number nine, continuing their consecutive run of top ten singles. In May and June 2008, Girls Aloud embarked on the Tangled Up Tour—their third arena tour, and fourth overall. They played a total of 34 concerts around the UK, including 24 arenas and 11 open air venues, making this tour their longest yet. They were scheduled to play 13 open air venues, but due to the bad weather, two of the concerts were cancelled. The girls also appeared as special guests at Kanye West's Glow in the Dark tour.

In May 2008, the group confirmed that they had begun working on their fifth studio album. The first single from the album, "The Promise", was released in October 2008, followed by the album, Out of Control, on 3 November. Girls Aloud said that it was their "most exciting and thrilling album yet". "The Promise" became their fourth number one on the UK Singles Chart, selling more than 77,000 singles in its first week of release—this made it the fastest selling single of 2008 up to that point. Out of Control followed suit when it entered at number one on the UK Albums Chart. The single returned the group to the top two on the Irish Singles Chart, while the album became their first top ten on the Irish Albums Chart since Sound of the Underground. "The Loving Kind" was released as the album's second single on 12 January 2009. The song, co-written by Pet Shop Boys became the girls' twentieth consecutive top ten single., charting at number ten.

Girls Aloud also performed at the BRIT Awards for the first time in their careers in 2009. They were nominated for Best British Group and Best British Single ("The Promise"). They won the award for Best Single, their first ever BRIT Award but lost out to Elbow for Best British Group. The Out of Control Tour is scheduled to commence in April, and Girls Aloud will support Coldplay at Wembley Stadium on 18 September 2009.

In February 2009, it was announced that Girls Aloud had signed a new record deal with Fascination which will see the group release another three albums, with the next album being released in Autumn 2010. Girls Aloud are also set to release Out of Control in continental Europe in the near future, with a television advertisement tie-in in Germany.

"Untouchable" was the third single from the album. The song was released in April to coincide with the Out of Control Tour, and peaked at number 11 in the UK Singles Chart.

In April 2009, it was announced that a singles boxset collection would be released. The boxset contains all 21 singles (making up 150 tracks and 13 hours of music), 16 videos, 8 games, an exclusive rarities disc and a 64 page booklet featuring the story behind the music. Sarah Harding announced in July 2009 on Alan Carr: Chatty Man that the girls are taking a break from music to concentrate on solo projects. She also announced the band aren't splitting and that they will release a new album in late 2010.

Despite many split rumours Girls Aloud have denied these allegations. They stated that although they are currently working on solo projects this will co-exist with being in the band and with the new record deal signed they will be recording a minimum of three more albums. In saying this they have assured the fans that they will be back in the studio and a new album will be released in 2010.