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Sienna made her film début with South Kensington, with Rupert Everett and Elle Macpherson and later had a regular 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 adaptation 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.