Nayantara's portrayal of Keerthi was appreciated by critics. Her first release, the family entertainer Yaaradi Nee Mohini was critically acclaimed and one of the highest grossing Tamil films of the year. In 2008 she had five releases, four of which were in Tamil. Similarly a critic from noted that she looked "great in mini skirts, jacket, dark glasses and tall boots".
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The reviewer further wrote: "Nayanthara has go full throttle to look her sexiest best She has a beautiful body which she flaunts daringly and is also able to bring out the cold aloofness and bitterness of her character. Sify heaped praise on her, describing her as a "show stopper". A remake of the same-titled 1980 Tamil film, it went on to become a blockbuster success at the box office, while Nayantara received many accolades for her performance as Sasha in her new glamour look. She regained her star billing in Kollywood acting opposite Ajith Kumar in the Vishnuvardhan-directed gangster film Billa (2007). In Thalaimagan, she played a news reporter, with critics agreeing that she did not have much to do in the film. Reviewers claimed that she made an impact, was "very adequate and impressive in a slightly complicated role", and that she had "come up with a good performance". The science fiction thriller E featured Nayantara in the role of a bar dancer. She looks gorgeous especially in songs and does justice to her well-etched out role". Sify wrote: "Nayanthara virtually walks away with the film and has never looked so beautiful. In Vallavan, she portrayed a lecturer who falls in love with a student younger than her. All three films opened to mixed reviews Nayantara mostly won praise for her performances. Three Tamil films in which she enacted the lead female characters – Vallavan, Thalaimagan and E – were released simultaneously during Diwali 2006. She next made her debut in Telugu, starring in the film Lakshmi, following which she performed in Boss, I Love You, alongside Venkatesh and Nagarjuna respectively. termed her performance as the "strength of the movie". Her first release in 2006 was Kalvanin Kadhali. Nayantara then accepted to appear in an item number as herself in the Perarasu-directedmasala film Sivakasi starring Vijay. However, she later told that appearing in Ghajini was a big mistake and the "worst decision" she ever took. Murugadoss' Ghajini, in which she played a secondary female character, again was a commercially highly successful venture. Later that year her third Tamil film, A. The film became one of the most successful Tamil films in history, running for over 800 days in theatres, eventually turning Nayantara into one of the most-sought after actresses in Tamil. Vasu's wife had seen Manassinakkare and recommended her. While still shooting for Ayya, she was selected to portray the love interest ofRajinikanth in the comedy horror film Chandramukhi, after its director P. claimed that she had made a "sensational debut in Tamil", while a reviewer from said that her "presence with her beautiful smile is crowd winning".
The family drama film opened to positive critical response, fetching Nayantara positive feedback as well. In 2005, she was cast opposite Sarath Kumar in Hari's Ayya, debuting in the Tamil film industry. She subsequently started appearing in Tamil and Telugu films. Work in Tamil and Telugu cinema (2005–09) She also acted opposite Mammootty in Thaskara Veeran and Rappakal. Her performance in Vismayathumbathu, in particular, was lauded, with critics claiming that she had "stolen the thunder with her author-backed role", and was "the revelation of the film". Her both releases in 2004, Natturajavu by Shaji Kailas and Fazil's psychological thriller Vismayathumbathu saw her co-starring alongside Mohanlal while she played the protagonist's adopted sister in the former, she portrayed a ghost in the latter. Manassinakkare went on to become a high financial success and she continued to receive acting offers. Although she turned down the offer initially, as she was not interested in films, she gave in eventually and agreed to do "just that one movie". She was spotted by director Sathyan Anthikkad, who had seen some of her modelling assignments and approached her to play a pivotal role opposite Jayaram in his film Manassinakkare (2003). While studying at college, Nayantara was working as a part-time model.