She made her acting debut with Ab Ke Baras (2002), but gained recognition only after the success of her 2003 film, Ishq Vishk, in which her portrayal as Payal earned her the girl-next door image. Success followed for her in 2004 with films like Masti and Main Hoon Na.

Her career took a setback when her following releases, Deewaar (2004), Vaah! Life Ho To Aisi (2005), Shikhar (2005), and Pyare Mohan (2006) did poorly at the box office. Things turned around when she starred in Sooraj R. Barjatya's blockbuster Vivah (2006) opposite Shahid Kapoor. The film was a universal success and her performance was well appreciated by critics, earning her a Dadasaheb Phalke Academy Award.

Rao recently made her debut in Tollywood, with the Telugu hit Athidhi opposite Mahesh Babu. Amrita had no releases in Bollywood in 2007. Amrita's first release of 2008 was My Name Is Anthony Gonsalves , which failed at the box office. Her performance got poor reviews.