Born in a theatre in New York City, Miller moved to London with her family when she was just over a year old. Her mother, Josephine, is a South African-born former model. Her father, Edwin Miller, is an American banker turned dealer of Chinese art. Miller has a sister, Savannah, and two half-brothers, Charles and Stephen. Miller attended Heathfield St Mary's School, a boarding school in Ascot, Berkshire, and later studied for a year at the Lee Strasberg Institute in New York City. She carries both British and American passports, and acquired her first driving licence in the US Virgin Islands, as it was easier to qualify there, thus allowing her to drive in both the US and UK.
Prior to her professional acting career, Miller worked as a photographic model. She signed with Tandy Anderson of Select Model Management London, and modelled for Coca-Cola, Italian Vogue, and posed topless in the 2003 Pirelli Calendar. Miller has also been closely associated with the style of fashion that became known as boho chic, much of which fashion followers noted was strikingly similar to the style of model Kate Moss. Miller signed a two-year contract with Pepe Jeans London; the jeans ad campaign first appeared in magazines March 2006. In February 2009, Hugo Boss Fragrances announced that Miller would be the new ambassador for their women's BOSS Orange women's perfume.
In 2001, she made her film début with South Kensington, with Rupert Everett and Elle Macpherson and later had a recurring role in the television drama series Keen Eddie. In 2004 Miller had a supporting role in the remake Alfie with Jude Law and in Layer Cake. In 2005, Miller played the female lead opposite Heath Ledger in the period comedy drama, Casanova, followed by the role of 1960s socialite and Andy Warhol's muse Edie Sedgwick in Factory Girl, which opened 29 December 2006. In 2007, Miller had a small role in Matthew Vaughn's adaption Stardust and played a starlet to Steve Buscemi's reporter in Interview, another remake. Later in 2007, she portrayed an undead bride opposite James Franco in Camille.
In 2008, Miller appeared in the film version of writer Michael Chabon's novel, The Mysteries of Pittsburgh and filmed The Edge of Love, with friend Keira Knightley, a biopic of Dylan Thomas in which she plays his wife Caitlin. She appeared in the 2009 live-action film adaptation of the comic book and cartoon G.I. Joe, G.I. Joe: The Rise of Cobra, playing The Baroness. She appeared in the film Hippie Hippie Shake a Working Title production which starred Cillian Murphy and played the title role in Patrick Marber's After Miss Julie on Broadway. She starred as Patricia in the London production of Flare Path at the Theatre Royal Haymarket in 2011.
In 2006, it was announced that Miller would design a fashion capsule for Pepe Jeans; the project was later expanded to become a complete fashion label. Called Twenty8Twelve, it gets its name from Miller's date of birth and is financially backed by Pepe Jeans. The collection, which Miller designed with her sister Savannah, a professional fashion designer, launched in September 2007.
Miller is the Global Ambassador for International Medical Corps. She traveled with them to the Democratic Republic of the Congo in April 2009, and kept a blog about her experiences. She also visited Haiti with the group after the 2010 Haiti earthquake. Miller also worked alongside Global Cool during their 2007 eco friendly campaign.
Miller is an ambassador for the UK branch of the Starlight Children's Foundation, which works with seriously ill children and their parents.
Miller's relationship with Alfie co-star Jude Law was scrutinised by the tabloid press. On Christmas Day 2004, they became engaged. On 8 July 2005, Law issued a public apology to Miller for having an affair with the nanny of his children. After attempting to salvage their relationship, Miller and Law separated in November 2006.
In 2008, Miller had a highly publicized affair with married actor Balthazar Getty. Miller later sued two British tabloids over the publication of photos showing her and Getty together.
In December 2009, it was reported that Law and Miller had rekindled their relationship after starring in separate shows on Broadway in late 2009. They spent Christmas 2009 in Barbados, along with three of Law's children. They announced they had split again in February 2011.
She has been dating actor Tom Sturridge since 2011 and together they have a daughter, Marlowe, born in July 2012. They are currently engaged.
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