In the 2000s and 2010s, she was known for her work in the thriller and horror genres and for several item numbers, and was frequently cited in the media as a sex symbol and a scream queen.

[11] She finally made her acting debut in a negative role opposite Akshay Kumar in Abbas–Mustan's action thriller Ajnabee (2001) which also starred Kapoor and Bobby Deol.

[16] Ajnabee received mixed reviews from critics upon release, with particular praise for Basu's performance, and it emerged as a moderate commercial success at the box-office.

[22] She next starred in Sanjay Gadhvi's romantic comedy Mere Yaar Ki Shaadi Hai (2002) alongside Uday Chopra, Jimmy Sheirgill and debutante Tulip Joshi.

It opened to mixed reviews from critics upon release, with praise for Basu's performance, and emerged as a moderate commercial success at the box office.

[23] Her next film that year, David Dhawan's action comedy Chor Machaaye Shor alongside Deol, emerged as her first critical and commercial failure.

[26] In 2003, Basu starred in Pooja Bhatt's erotic thriller Jism alongside debutant John Abraham, in which she portrayed the seductive, ambitious wife of a millionaire, who indulges in an extramarital affair with an alcoholic lawyer and plots to kill her husband.

It received mixed reviews upon release, but Basu earned praise for her portrayal of a femme fatale, with Taran Adarsh of Bollywood Hungama commenting, "...the real show stealer is Basu; her sexy look and seductive deep voice, in contrast with her cold and calculating personality, makes her the most impressive femme fatale since Zeenat Aman and Parveen Babi.

However her next release, Rohit Shetty's directorial debut Zameen alongside Ajay Devgn and Abhishek Bachchan, emerged as a critical and commercial failure.

She then appeared in Prakash Jha's crime action film Apaharan, alongside Devgn and Nana Patekar, which was a critical and commercial success.

[42] Basu established herself as a leading actress of Hindi cinema in 2005 and 2006 with the progressive success of the comedy No Entry, the drama Corporate and the action thriller Dhoom 2.

[47] In Madhur Bhandarkar's Corporate, she gave up her glamorous look to portray a businesswoman who has no qualms in taking advantage of her sexuality to con the CEO of a rival company.

[49] In Vishal Bhardwaj's adaptation of Othello, Omkara, Basu played the role of Billo Chamanbahar (Bianca), alongside an ensemble cast of Devgn, Kareena Kapoor, Saif Ali Khan, Konkona Sen Sharma and Vivek Oberoi.

[50] Moreover, her performance also earned positive reviews, with critic Rajeev Masand of CNN-IBN writing, "...Basu is brought in to lend oomph and she highly succeeds in doing that.

[52] The film, and Basu's performance, received positive reviews from critics upon release, with Nikhat Kazmi of The Times of India commenting, "Aah Bipasha!

"[59] Basu next starred alongside Ranbir Kapoor, Deepika Padukone and Minissha Lamba in Siddharth Anand's romantic comedy Bachna Ae Haseeno as a successful supermodel who finds it hard to forgive her ex-lover for betraying her.

[citation needed] She was then featured as a Kashmiri girl alongside Sanjay Dutt, Anupam Kher and Kunal Kapoor in Rahul Dholakia's drama thriller Lamhaa, which explored socio-political problems in Kashmir.

NDTV Movies wrote, "Basu sinks herself into her character imparting a dramatic resonance into the role without resorting to stock expressions.

"[71] Basu's next appearance that year was in Priyadarshan's action thriller Aakrosh as the wife of a ruthless cop who helps the police investigating honor killings in their village.

Nikhat Kazmi of The Times of India commented, "Basu actually doesn't have much to do and does seem to be miscast as the much-abused, bruised and battered wife of Paresh Rawal".

[79] Majorly hyped prior to release, Players was a commercial disaster at the box office, and was negatively compared to The Italian Job and highly criticised for its execution and performances, including that of Basu.

Co-starring Emraan Hashmi and Esha Gupta, the film proved a major commercial success at the box office, grossing ₹1.01 billion (US$12 million) worldwide.

"[82][83] After a guest appearance in Race 2 (2013) where she reprised her role from the prequel,[84][85] Basu starred alongside Nawazuddin Siddiqui in the horror film Aatma directed by Suparn Verma.

[86][87][88] Basu next performed live alongside Atif Aslam, Shaan and Malaika Arora for the first time in a series of concerts in Birmingham and London[89] in the summer of 2013.

Basu didn't even participate in the film's promotions because she was "extremely disturbed by the result" and stated, "Humshakals was the worst experience of my life".

[94] The same year, Basu finished shooting for her first English film project, Roland Joffé's Belgian romance time travel adventure The Lovers, in which she portrayed a Maratha warrior.

[97] The film performed moderately well at the box office, and received mixed reviews from critics upon release, with praise for Basu's dual role.

[98] India TV reviewed the film and wrote that, "With some genuine scary moments and Basu-Grover's scorching chemistry, Alone stands apart from numerous horrible horror flicks made in the past," and also stated, "Basu just takes her act to another level.

[citation needed] Hiren Gada, director of Shemaroo Entertainment, said, "A celebrity like Basu, genuinely believes in staying healthy.

[114][115] In January 2014, Basu launched the third instalment of her Love Yourself DVD fitness series, Unleash, an advanced training routine including plyometrics and focusing more on power and speed, while strengthening the bones and improving muscle coordination.