Harmon began acting in 1995 after being discovered on a plane by David Hasselhoff. She then starred in several television series, including Baywatch Nights, Baywatch and C-16: FBI; she also appeared in the 1998 film, Lawn Dogs, which received only a limited theatrical release. In the early 2000s, Harmon became better known as playing Abbie Carmichael on the series Law & Order, a role she played from 1998 to 2001. During this time, she also voiced Barbara Gordon in the animated film, Batman Beyond: Return of the Joker, replacing Stockard Channing, as well as appearing on Law & Order.
Harmon left Law & Order to concentrate on her film career, saying that she preferred working in film than television. After appearing in the 2001 direct-to-video film Good Advice, she had a major role in Agent Cody Banks, playing the CIA handler of a teenage agent (Frankie Muniz). The film opened in March 2003 and became a minor hit, grossing $47 million. Although Harmon was originally scheduled to appear in the sequel, the producers chose to take a more comedic approach, and replaced Harmon with Anthony Anderson. In 2006, Harmon co-starred with Cuba Gooding Jr. and James Woods in the direct-to-DVD political suspense drama End Game.
In 2006, Harmon starred as the lead in the ABC pilot Secrets of a Small Town. Despite testing highly with focus groups, the pilot was not picked up by ABC due to its high budget. She also starred in another failed television show on NBC, Inconceivable. The program was canceled after two episodes. In 2007, she starred in another ABC pilot, Women's Murder Club. The police drama was picked up, but cancelled after the first season with only 13 episodes produced and aired. In April 2008 Angie Harmon Goes Naked for Allure Magazine is among five actresses who strip down to their birthday suits for the May issue of Allure magazine. She appears nude along with Gabrielle Union; Zoe McLellan (of ABC's "Dirty Sexy Money"); singer and actress Jill Scott; and "Ugly Betty" co-star Ana Ortiz.