Their fourth album Seventh Tree placed a greater emphasis on ambient and downtempo music, drawing inspiration from nature and Paganism, while their fifth album, Head First, found the group exploring 1980s-influenced synthpop. Head First also earned the duo their second Grammy Award nomination for Best Electronic/Dance Album in 2010. Goldfrapp are scheduled to release their sixth studio album in 2013.

Alison Goldfrapp began her musical career in the early 1990s as a guest vocalist with the electronic band Orbital and trip hop artist Tricky. In 1999, she was introduced to composer Will Gregory after he had listened to an early version of the song "Human". Gregory felt a connection with Goldfrapp and invited her to record a demo for the film soundtrack he was composing, to see if they could work together. The demo was never completed, but the recording session had been pleasant. Following several months of phone calls, they decided to form a musical band and began performing under Goldfrapp's last name.

In August 1999, Goldfrapp signed a recording contract with London-based record label Mute Records. The pair began recording their debut album over a six-month period, beginning in September 1999, in a rented bungalow in the Wiltshire countryside. The recording process was difficult for Alison, who often found herself alone and disturbed by the mice and insects in the bungalow.

Goldfrapp's debut album Felt Mountain was released in September 2000 and produced the singles "Lovely Head", "Utopia", "Pilots (On a Star)" and "Human". The album featured Alison Goldfrapp's synthesised vocals over cinematic soundscapes and is influenced by a variety of music styles including cabaret, folk and electronic music. The album was well received by music critics, which Pitchfork Media described as "simultaneously smarmy and seductive, yet elegant and graceful". It reached number 57 on the UK Albums Chart, and was certified gold by the British Phonographic Industry. In 2001, Felt Mountain was shortlisted for the Mercury Prize, an annual music prize awarded for the best British or Irish album from the previous year.

The lyrics on Felt Mountain were written by Alison Goldfrapp and are abstract obsessional tales inspired by films, her childhood, and the loneliness she felt while recording the album. The song "Oompa Radar" was inspired by Roman Polanski's film Cul-de-sac, while "Pilots", which describes travellers floating in the atmosphere above the earth, was inspired by John Barry's James Bond theme songs.

To promote Felt Mountain, Goldfrapp toured the UK, Europe and North America, supporting the alternative music bands Nick Cave and the Bad Seeds and The Doves. The band found it difficult to perform songs from the album live because of their complex arrangements which required up to forty musicians. They eventually settled on performing with violinist Davide Rossi, drummer Rowan Oliver and keyboardist Andy Davies.

Goldfrapp's second album Black Cherry was released in April 2003. The band recorded the album in a darkened studio in Bath, England. The studio's walls were covered in neon lights and Goldfrapp used them to write down her song ideas. The album focused more heavily on dance music and glam rock-inspired synths than its predecessor. Alison Goldfrapp commented that the album differed from Felt Mountain because the band "felt that we really didn't want to repeat what we had done...we kind of wanted to do something that felt equally as fresh to us as the first one felt fresh to us, and we wanted to put more kind of "oomph" in it." The album received positive reviews from critics. The Guardian found it to be an "unexpected delight" and About.com called it a "rare electronica album of warmth and depth...the ultimate chillout pleasure". Black Cherry peaked at number 19 on the UK Albums Chart and number four on the Billboard Top Electronic Albums chart in the United States. It sold well, reaching platinum status in the UK and selling 52,000 copies in the US as of August 2006.

The first single released from the album was "Train", which reached number 23 on the UK Singles Chart. The song's lyrics discuss obsession and overindulgence and were inspired by Goldfrapp's visit to Los Angeles while touring in support of Felt Mountain. "Strict Machine" was released as the album's second single. The song proved successful on several formats, and reached number one on the US Hot Dance Club Play chart. In 2004, "Strict Machine" won an Ivor Novello Award for "Best Dance Single". The third single released from Black Cherry was "Twist", a song inspired by a sexual fantasy Goldfrapp had as a teenager. The title track was released as the album's fourth single and reached number 28 in the UK.

In 2003, Alison Goldfrapp modified her image, from a sophisticated Marlene Dietrich inspired look to that of a New Wave diva. The reinvented image included false eyelashes, customised T-shirts, military uniforms and fishnet stockings. Starting in March 2003, the band toured the album, with a concert series entitled Black Cherry Tour. In 2004, the band further toured Australia, Japan, Europe and North America supporting Duran Duran, and embarked on the Wonderful Electric Tour. Sections of the stage show featured Goldfrapp in a white dress wearing a horse tail and dancers with deer heads, and were inspired by Goldfrapp's interest in animals and mythology.

Supernature, Goldfrapp's third album, was released in August 2005. The album comprises pop and electronic dance music prominently featured on Black Cherry, but focuses more on subtle hooks instead of the large choruses that made up its predecessor. The band never intended to create dance music, however, previous releases were popular across nightclubs in North America and as a result, they decided to write a more dance-oriented album. Supernature debuted at number two on the UK Albums Chart and was certified platinum in the UK. As of February 2008, it has sold one million copies worldwide. The album received a Grammy Award nomination in 2007 for Best Electronic/Dance Album and "Ooh La La" was nominated for Best Dance Recording.

"Ooh La La", the album's lead single, became Goldfrapp's first UK top five single. The song was chosen as the lead single "because it was up and in your face and carried on the theme of the glammy, discoey beat from the last album". "Ooh La La" became the first song performed by the band to feature the electric guitar and was often cited as a highlight of the album by Allmusic. "Number 1" was released as the album's second single. Constructed around a synthesiser and bass arrangement, it was written about the importance of relationships. The album's third single "Ride a White Horse" was inspired by the disco era and reached number 15 in the UK. "Fly Me Away" was released as the album's fourth single, but did not perform as well as its predecessors.

In 2006, Goldfrapp released We Are Glitter, a North American-only compilation of remixes from Supernature. It included a Flaming Lips remix of "Satin Chic", the band's favourite song from the album.

Goldfrapp began writing and recording their fourth album at the end of 2006 in Bath, England. Alison Goldfrapp described their winter recording sessions as difficult. However, spring recording sessions brought them more favourable results. Seventh Tree, their fourth album, was released in February 2008, and debuted at number two on the UK Albums Chart. The album is a departure from the pop and electronic-dance music featured on Supernature, and features ambient and downtempo music. The band were inspired by an acoustic radio session they had performed, which led the duo to incorporate acoustic guitars into their music to create "warm" and "delicate" sounds.

The album's lead single, "A&E", reached number ten in the UK. The single received positive reviews from critics, musicOMH found it to be "a beautifully paced ballad" and Digital Spy called it "lush, folky and organic". "Happiness", the album's second single, reached number 25 in the UK. The third single, "Caravan Girl", which describes the story of a girl that suffers from amnesia, reached number 54 in the UK.

In 2008, Alison Goldfrapp again reinvented her image, this time as a circus performer. The artwork for Seventh Tree featured her dressed as a clown because it is an "iconic image" with "so many different connotations". Goldfrapp chose to tone down her overtly sexual image because she felt that it was taking over the music. Her new image, inspired by Paganism, featured her dressed in white or natural-coloured flowing gowns with loose, curly blond hair.

Goldfrapp's fifth album, Head First, was released in March 2010. Recorded over a six-month period, it was a return to the dance oriented sound on previous albums. The album took inspiration from 1980s pop music and bands such as Van Halen and The Pointer Sisters. Alison Goldfrapp described its sound as "optimistic and vibrant." The album received positive reviews from critics, with Allmusic describing it as "a love letter to the frothy, fleeting, but very vital joys of pop music." Head First peaked at number six on the UK Albums Chart and number 45 on the US Billboard 200. The album earned Goldfrapp a Grammy Award nomination in 2011 for Best Electronic/Dance Album and "Rocket" was nominated for Best Dance Recording.

The album's first single was "Rocket", a song about an unfaithful lover. Musically, The Times and Spin have compared the song to "Jump" by American rock band Van Halen. In the US, "Rocket" peaked at number one on the US Hot Dance Club Play chart. "Alive" was released as the album's second single. The song's music video featured Alison Goldfrapp as a 1980s inspired aerobics instructor who leads a group of black metal fans and vampires through a fitness routine. The album's third single "Believer" featured remixes by Vince Clarke and Davide Rossi.

In February 2012, Goldfrapp released the compilation album The Singles. The album contained previously released material as well as two newly recorded songs. Goldfrapp's sixth studio album is scheduled to be released in 2013.

Although Goldfrapp's musical style has changed over time, it is considered to be an electronic music act. Goldfrapp has explored a range of musical styles in their songs, although many songs are characterised by Alison Goldfrapp's distinctive breathy, soft soprano vocals and Will Gregory's multi-layered synthesiser and string arrangements. The band's sound has progressed from an ambient sound in Felt Mountain, through electronic music in Black Cherry to a more glam rock influence in Supernature, and most recently to a blend of ambient, folk and electronic in Seventh Tree and an 1980s synthpop influence in Head First. However, they have experimented with other genres of music, such as cabaret ("Cologne Cerrone Houdini", "Oompah Radar"), folktronica ("A&E") and trip hop ("Little Bird").

Goldfrapp draws inspiration from a range of artists and genres. Alison Goldfrapp listened to Kate Bush, T. Rex, Donna Summer and Iggy Pop as a teenager and discovered Serge Gainsbourg while working in Belgium. While travelling through Europe in the early 1990s, she also began listening to Polish disco music and cabaret music from the Weimar Republic. Will Gregory's musical background was classical music and has cited Ennio Morricone as his main influence. Other media, including film, have had an impact on Goldfrapp; Alison Goldfrapp cites Roman Polanski's psychological thriller Cul-de-sac, the cult film The Wicker Man, and the James Bond franchise as influences. They also draw inspiration from surrealism and nature, all of which appear in the band's album artwork, which Goldfrapp designs in collaboration with Big Active.

The majority of the band's songs are composed by Goldfrapp and Gregory, although they have collaborated with session musician Nick Batt several times. They have called their writing relationship a "democracy", playing off one another while in the recording studio. However, Goldfrapp is responsible for the lyrics. While writing, Goldfrapp uses her vocals to create melodies and drumbeats. Gregory composes his music on vintage keyboards, interpreting the mood of Goldfrapp's lyrics. Alison Goldfrapp believes that "music is a visual experience" and therefore visualises her lyrics before writing them. Her songwriting is characterised by its use of animals to describe human emotions and status.