In 2012, she made her film debut as Éponine in the film version of the long-running musical Les Misérables.

For the film, she received nominations for the Screen Actors Guild Award for Outstanding Performance by a Cast in a Motion Picture, Satellite Award for Best Supporting Actress – Motion Picture, and Broadcast Film Critics Association Award for Best Acting Ensemble, and won the National Board of Review Award for Best Cast and Empire Award for Best Female Newcomer.

n April 2007, Barks released her debut album, Looking in Your Eyes, which sold around 600 copies. The album featured several songs which she co-wrote herself and was released on the independent label Brunswick Studios. She also performed at the Peel Bay Festival in June 2007 supporting Matt Willis and the Sugababes, which also saw appearances by Madness and The Who. In December 2007, Barks represented the Isle of Man in the Maltese International Song Competition where she won the main prize of €2000 and the title of Best Foreign Singer. She sang the song "Nothing Else" from her album and "Play On", a hit song in Malta

In 2008, Barks competed in I'd Do Anything in which she was one of the finalists in a search for a new, unknown lead to play Nancy in a West End revival of the British musical Oliver!. She reached the final where she finished third. On 29 April 2008, the Isle of Man was renamed by the Tourism Minister Adrian Earnshaw to be the "Isle of Sam" as a sign of support. Welcoming signs at Ronaldsway Airport and Douglas Sea Terminal were changed after a renaming ceremony

In week eight of the show, she performed "Defying Gravity" from the musical Wicked and in the week leading up to the show she was given support from American actress Idina Menzel who achieved fame for her performances as Elphaba, the Wicked Witch of the West in Wicked.

In week nine, Barks received the lowest number of public votes and so had to participate in the sing-off with Rachel Tucker. They sang "Memory" from the musical Cats. Andrew Lloyd Webber chose to save Barks and eliminate Tucker saying, "Last night Cameron and I were both saying that we thought both of you would be fantastic Nancys and now here am I faced with this. But I've got to make a decision and I've got to think of where the show ultimately for Cameron is going to go and I think I have to go with you, Samantha."

In the week leading up to the final shows on 31 May, the Nancy finalists posed for publicity pictures recreating some of Madonna's iconic images. Barks was dressed in hotpants copying the pose from the cover of the 2008 album, Hard Candy. Each Nancy also had a "Master Class" with Liza Minnelli in London.

Samantha Barks in 2011 At the end of Show one of the final, Barks was announced as finishing third with Andrew Lloyd Webber saying, "Do you know what, I did think this would happen. But you've done so well to have got this far, Samantha." Barks said, "It's been the most amazing experience of my life. Thanks to everyone and the panel for making it so incredible.

Barks reprised her role as Éponine in the 2012 film adaptation of Les Misérables. She learned the news from Cameron Mackintosh during an Oliver! curtain call.

During filming for Les Misérables, Barks recorded the song "Defective" for the album Scott Alan Live which was released in December 2012.

In June 2012, just days after completing Les Misérables, Barks returned to the UK tour of Oliver! for two weeks at the Edinburgh Playhouse.

On 24 June 2012, Barks performed in a Little Women charity concert at the Playhouse Theatre in London.

On 13 October 2012, Barks performed at the Indoor Garden Party concert in New York City's Gramercy Theatre. The concert was part of a concert series created by Russell Crowe and Alan Doyle.

Barks performed at another Indoor Garden Party concert at New York City's Joe's Pub on 8 December.In early November 2012, Barks briefly returned to the Oliver! UK tour at the Grand Theatre, Leeds. Barks permanently returned to the Oliver! on 12 December at Bord Gáis Energy Theatre in Ireland and continued with the tour until 20 February 2013 at the Bristol Hippodrome.

She left the show early in order to head to Los Angeles for rehearsals with fellow Les Mis co-stars for their cast performance at the Oscars on 24 February 2013. Her rendition of "On My Own" from Les Miserables reached number 97 on the Billboard Hot 100, and number 43 in the UK, being her first entry on each chart.

On 11 February 2013 Barks won Best Breakthrough Performance at the Elle Style Awards. Barks performed with her co-stars from the film Les Miserables at the 85th Academy Awards ceremony on 24 February 2013.

Immediately after the Oscars, Barks flew to the Isle of Man to begin work on her second film, The Christmas Candle

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