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While pursuing her studies in architecture, Rai began modelling on the side. In the 1994 Miss India contest, she won the second place behindSushmita Sen, and was crowned Miss India World. She went on to win the Miss World title the same year, where she also won the Miss Photogenic award. She abandoned her academic education after winning the pageant and spent one year reigning as Miss World in London. Rai then started working as a professional model and then moved on to her current profession as an actress.
Rai made her acting debut in Mani Ratnam's Tamil biopic film, Iruvar (1997) with Mohanlal, The controversial film was a critical success and won many awards including Best Film award at the Belgrade International Film Festival, two National Film Awards, and two Filmfare Awards South. Rai appeared in dual roles, opposite veteran actor Mohanlal, with one of her roles being a cinematic depiction of political leader and ex-actress J. Jayalalithaa. Rai made her Bollywood debut in the film, Aur Pyaar Ho Gaya opposite Bobby Deol, which also released that year; the film did not do well at the box office, and was also panned by critics. However, her third project, S. Shankar's Tamil film, Jeans(1998) was a commercial success. The film was also noted for the song "Poovukkul", written by Vairamuthu, in the lyrics of which, she is compared to the seven wonders of the world and described as the eighth.
Her re-entry to Telugu movies happened with a film with Sreekanth which was a failure; then in Sri Anjaneyam, directed by ace directorKrishna Vamsi which too was a failed attempt. It was followed by another failure with Chanti, paired against Ravi Teja. She finally got a big break in Telugu with Gowri in which she was paired with Sumanth. She didn't have to look back afterwards. The stupendous success of Masswith Nagarjuna strengthened her position in Tollywood. Charmme's most indistinguishable and critically acclaimed film so far is Anukokunda Oka Roju. It was a heroine-oriented thriller. Her performance in the movie was acclaimed by critics.
In 2006 she acted in Pournami which was a total failure in spite of high expectations, but her performance was appreciated. Though she did not learn Indian classical dance, her Bharatanatyam and Kuchipudi dances in the film were appreciated by audiences. Later that year she was paired for the second time with Sumanth in Chinnodu but it was not a successful venture. Her next film, Rakhi (with NTR), was a hit. In2007 Mantra, a thriller with Charmme in the lead role, was declared as a surprise hit.This performance fetched her the Nandi Award for the best herione of 2007. Her performance in the movie is appreciated by wide range of audience.
Then, she starred in several lady oriented roles, a rare thing in Tollywood. The list includes Anukokunda Oka Roju, Mantra, Manorama 2009,Kavya's Diary in Telugu and Laadam in Tamil, out of which Anukokunda Oka Roju and Mantra were very successful.