She was invited to tour with Jamie T after he attended her second solo gig. She has toured with a number of other musicians including Adam Green from the anti-folk band The Moldy Peaches. She performed at the 2007 O2 Wireless Festival and performed at the first Underage Festival in August 2007 at Victoria Park, East London, before releasing her debut EP “London Town” on WayOutWest Records.

Her debut album Alas, I Cannot Swim was released on 4 February 2008, and was nominated for the 2008 Mercury Prize. The album, as well as subsequent singles, were released on Virgin Records. The third and final single from her album, “Night Terror” was released on 27 October 2008, coinciding with a 6-date “Night Terror tour”.

Marling’s television appearances include The Late Late Show with Craig Ferguson and Later With Jools Holland, performing “Ghosts” and “New Romantic” respectively. In 2008, she appeared on Russell Brand’s Radio 2 show alongside her sister. She once chose to perform on the street after being denied entry to one of her own performances for being underage.

Marling dated Noah and the Whale singer/guitarist Charlie Fink briefly before the pair separated in 2008. She also dated Marcus Mumford of Mumford & Sons until late 2010. She moved to Silver Lake in Los Angeles, California in 2013, before relocating to London in December 2014.

The follow-up to Alas, I Cannot Swim, titled I Speak Because I Can, was released on 22 March 2010. Produced by Ethan Johns, the album has a more mature sound and lyricism, dealing with “responsibility, particularly the responsibility of womanhood”. The album is preceded by the singles “Goodbye England (Covered in Snow)”, released on iTunes in December 2009 and “Devil’s Spoke” on 15 March 2010. On 28 March 2010, I Speak Because I Can entered the UK Albums Chart at Number 4. It was nominated for the 2010 Mercury Music Prize. In 2013, NME listed the album at 263 in their list of the 500 greatest albums of all time.

Marling’s third album, A Creature I Don’t Know, was released on 12 September 2011. The album received positive reviews and reached number four on the UK album charts.

During October 2012, Marling completed the ‘Working Holiday Tour’ of the U.S. as a solo performer. At the time, she announced that the fourth album, later named Once I Was an Eagle, was finished and was scheduled for a February 2013 release; this was later delayed until May 2013. On 8 March 2013, Marling confirmed that the album would be released on 27 May 2013, and would be released in the U.S. one day later.

The fourth album’s first single “Master Hunter” was released on 17 April 2013, while Once I Was an Eagle entered the UK charts at number 3.

In September 2013, Marling explained: “I am a solitary person but I love people, I’m not a misanthrope. I like the idea of speaking only when it’s strictly necessary. The closest I ever feel to people is in shared experience. I’m still exploring that, I don’t know where it’s going to lead me.”

On 16 December 2014, Marling announced that her fifth studio album would be titled Short Movie, and its title track, released on the same date, is the lead single and was made available for digital download. The album features 13 songs composed by Marling and was released in the UK on 23 March 2015 and one day later in the US.

In October 2015, Marling announced a short Tour de Ville through the U.S., where she would be previewing material from her forthcoming sixth studio album.

Marling co-stars in the short film, “Woman Driver”, which was filmed in Marfa, Texas and directed by Chris Perkel. The movie was shot and edited in 72 hours. Marling later won “Best Actress” at the 72-Hour National Film Challenge. The film was shown at the London Short Film Festival on 14 January 2015 and later premiered on Vimeo the following month. The film also featured new music from Marling.

In a tweet, Blake Mills confirmed that Marling’s sixth studio album was completed. In November 2016, Marling announced the release of Semper Femina in March 2017, with “Soothing” the first single from the record. The album was released to critical acclaim. Marling received her first Grammy nomination for Best Folk Album for Semper Femina, but did not win the award. Semper Femina was also nominated for IMPALA’s European Album of the Year Award.

Marling covered “Red Right Hand” by Nick Cave and the Bad Seeds and “A Hard Rain’s a-Gonna Fall” by Bob Dylan for the season 4 finale of Peaky Blinders which aired on 20 December 2017.

In 2018, Marling announced that she would be recording an album with Mike Lindsay of the band Tunng, under the name LUMP. Prior to releasing an album, the duo released two singles, “Curse of the Contemporary” and “Late to the Flight”. On 1 June 2018, LUMP released its self-titled debut album. Marling provided the vocals and lyrics, while Lindsay played most of the instruments on the album.

On 5 April 2020, Marling announced the upcoming release of her seventh solo album via an Instagram, also releasing a song off the album, “Held Down”, at midnight. Song for Our Daughter was released on the 10 April 2020. The album, which had been set for release in August 2020, was released early, in part due to the COVID-19 pandemic. The pandemic also caused Marling to cancel many 2020 tour dates.

As of 2020, Marling is enrolled in a master’s degree program in psychoanalysis. She lives in northeast London with her boyfriend and older sister.