After receiving a diploma in filmmaking, she produced the small-budget caper-comedy Paisa Vasool (2004), in which she starred along with Sushmita Sen; this was probably the first ever chick-flick in Indian cinema in that it did not have a male lead nor a love story. Since then, she has played supporting and leading roles in various unsuccessful films, some of which being well received by critics, such as the historical epic drama Taj Mahal: An Eternal Love Story (2005), the thriller Tum - A Dangerous Obsession (2005), and the horror film Anjaane - The Unknown (2005). In Anwar, she played a supporting role along with her brother Siddharth, her only release in 2007. In 2008, she made her comeback to films, with her first leading role since Mumbai Express (2005), in Tulsi, opposite Irrfan Khan. Although before release, her comeback was described by the media as "shocking", and the film suffered from poor marketing, her performance as Tulsi, a young homemaker diagnosed with leukemia, was well received. Taran Adarsh from IndiaFM wrote: "Manisha Koirala sinks her teeth in this role and delivers a fine performance." She next starred in Sirf (2008). The film was released without any notice or publicity and was a critical and box office failure. Her first Bengali film Khela, directed by Rituparno Ghosh, released the same year, along with the long delayed Hindi film Mehbooba, both films released on the same day. In December 2009, she served as a Jury member in the fifth edition of the Dubai International Film Festival.

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In Anwar, she played a supporting role along with her brother Siddharth, her only release in 2007.