Dhanush's biggest film, in terms of budget, til date is the 2006-released Pudhupettai. The film, re-united him with his brother after their successful previous venture, pitted him against two prominent heroines Sneha and Sonia Agarwal. The movie is about the rites of passages in the life and times of an everyday-man who ends up as a dreaded gangster, 'Kokki' Kumar, the role portrayed by Dhanush. A critic praised Dhanush's relaistic portrayal, claiming that "as the innocent boy who transmogrifies into a bloody criminal, Dhanush is utterly believable. The subtle changes in his body language and his ability to give every expression a deeper meaning make the character more interesting. This is certainly one of his better performances." The film which became universally critically praised, failed to relate to Tamil Nadu audiences and ended up being an average grosser at the box-office, despite the positive reviews. The film fared marginally better, in the Telugu dubbed version, titled Dhoolpet. Dhanush achieved his first hit in three years with the commercial entertainer Thiruvilayadal Arambam, alongside Shriya Saran and Prakash Raj. The comedy film, showed the relationship between a poor man who loved the sister of a businessman. The film was well-received by critics and audiences alike.

Dhanush's first release of 2007, Parattai Engira Azhagu Sundaram, flopped at the box-office, gaining negative reviews in the process. The film, which was a remake of the successful Kannada language film, Jogi, starred him opposite Meera Jasmine However, his second film released during Diwali 2007, became a blockbuster at the box office, in which his performance was raved. Polladhavan, based on 1948-Italian neorealist The Bicycle Thieves, featured Dhanush opposite Divya Spandana, and the film's "fresh screenplay" by director Vetrimaran helped the film become a super hit.

The remake of a successful Telugu film directed by his brother, was the plotline for Dhanush's first 2008 release. Directed by debutant M. Jawahar, Yaaradi Nee Mohini with Nayantara became a big blockbuster at the box-office. He later appeared in a cameo appearance, for his father-in-law Rajnikanth's venture, Kuselan, being portrayed as himself in a song sequence. His latest venture was in Suraj's Padikathavan opposite Tamanna Bhatia which had a January 2009 release. His performance was praised, with Sify.com citing that "Dhanush is in top form in his dance" and "has improved a lot in action", with claims that the climax fight featuring him was "outstanding" and the film has become a super hit giving Dhanush a "hatrick successes". his last commercial hit wes Kutty opposite Shriya Saran. He is also acting in the film Aadu Kalam directed by Vetrimaran. He will also act in the remake of his father-in-law's yesteryear 1989 comedy flick Mappillai which has been given the same title. A film with Hari has also been announced, which is said to launch in July 2010