Jolie, who was the daughter of actor Jon Voight, spent much of her childhood in New York before relocating to Los Angeles at age 11. She attended the Lee Strasberg Theatre and Film Institute for two years and then enrolled at Beverly Hills High School. She later studied drama at New York University. In addition to acting in theatre productions, she modeled and appeared in music videos.

Jolie's first major movie role was in Hackers (1995), during the filming of which she met her first husband, British actor Johnny Lee Miller (married 1996; divorced 1999). The film failed to find an audience, as did a series of subsequent movies. In 1997, however, Jolie garnered much attention as the wife of Alabama's segregationist governor in the television movie George Wallace, and she later won a Golden Globe Award for her portrayal. The following year she played a supermodel struggling with drug addiction in the HBO movie Gia, a performance that earned her multiple honours, including a Golden Globe and a Screen Actors Guild Award. In 1999 she appeared in the comedy Pushing Tin with John Cusack and Billy Bob Thornton, and the following year she married Thornton (divorced 2003).

After her Oscar-winning turn in Girl Interrupted, Jolie starred in a series of action movies. She played the girlfriend of a carjacker (Nicholas Cage (Cage, Nicolas)) in Gone in Sixty Seconds (2000) and later adopted a British accent as well as mastering street fighting and kickboxing for the title roles in Lara Croft: Tomb Raider (2001) and Lara Croft Tomb Raider: The Cradle of Life (2003). In 2004 she portrayed the mother of Alexander the Great in Oliver Stone's Alexander and also starred opposite Gwyneth Paltrow and Jude Law in Sky Captain and the World of Tomorrow, a sci-fi thriller set in 1930s New York City. Both films were box-office disappointments, but Jolie scored a hit with Mr. & Mrs. Smith (2005), in which she played an assassin pretending to be a normal housewife; while working on the film, she met Brad Pitt, who became her partner. In Robert De Niro (De Niro, Robert)'s The Good Shepherd (2006), she was the aggrieved wife of an early CIA agent (Matt Damon (Damon, Matt)). Jolie earned critical acclaim for her performance as Mariane Pearl in A Mighty Heart (2007). Based on a true story, the film followed efforts to rescue Pearl's husband, Daniel, who was kidnapped and later murdered by Islamic extremists while reporting in Pakistan for The Wall Street Journal. Jolie's later films include Beowulf (2007) and Wanted (2008). Her immersion into the role of a mother whose son is kidnapped and later replaced by a different child in Clint Eastwood (Eastwood, Clint)'s Changeling (2008) resulted in another Oscar nomination.