Her sixth record, Semper Femina, was also nominated for a Grammy Award in the Best Folk Album category, as was Song for Our Daughter.

[8][11] After completing her GCSEs at age 16, Marling joined her older sisters and settled in the outskirts of London.

[12] She soon joined a cluster of intertwined bands that were drawn to acoustic instruments and tradition-tinged melodies—the group formed a musical movement that was labelled "nu-folk" by the British press.

[9] Marling joined the original line-up of indie folk band Noah and the Whale[10] and appears as a background vocalist on their debut album, Peaceful, the World Lays Me Down; however, she left the group before the album's 2008 release due to a dissolved relationship with the band's lead singer, Charlie Fink.

[8][13] Marling appeared on The Rakes track "Suspicious Eyes" from the band's 2007 album, Ten New Messages, credited as 'Laura Marlin'.

Marling later collaborated with Mystery Jets and contributed guest vocals to their 2008 single "Young Love".

She has toured with a number of other musicians including Adam Green from the anti-folk band The Moldy Peaches.

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;[25] this was later delayed until May 2013.

[26] Marling's fourth album's first single, "Master Hunter", was released on 17 April 2013,[27] while Once I Was an Eagle entered the UK charts at number 3.

[32] Marling revealed in a September 2013 interview that she had enough songs for a fifth album at the time, and she will "maybe make this record and then have a big, long, hard think about what I've done".

During a February 2014 performance for NPR's eTown series, Marling played one of the new songs, titled "Born to Love".

[34] Marling began recording songs for the album shortly after completing the solo tour for Once I Was an Eagle.

However, after recording a new album, she felt unsatisfied with the result, and made the decision to scrap most of the songs written in that period.

Both "False Hope" and "Short Movie" were received with critical acclaim,[37] many reviewers noting the larger sound and the confidence in Marling's vocals.

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

[44] 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.

Marling duetted with the Radiohead guitarist Ed O'Brien on "Cloak of the Night" on his debut solo album, Earth, released in 2020.

[53] On 5 April, Marling announced her seventh solo album via an Instagram post, and released a song, "Held Down", at midnight.

[60] On 5 May 2021, Marling announced the follow-up album to her collaboration with Mike Lindsay as Lump, entitled Animal, along with the release of the lead single of the same name.

[62] Following the birth of her daughter in 2023, Marling began writing and recording her eighth album, Patterns In Repeat, in London.

[65] She moved to Silver Lake in Los Angeles, California, in 2013,[66] before relocating to London in December 2014, after purchasing her first home.