With the support and encouragement of her husband and father-in-law, Indira accepted the offer to act in films and adopted Moushumi as her screen name.

[3] Chatterjee made her film debut as a child heroine in the Bengali hit Balika Badhu (1967), directed by Tarun Majumdar[4] when she was a preteen.

In an interview, Moushumi Chatterjee quoted: "After Balika Badhu, I was flooded with Bengali movies but I wished to complete my studies.

"[4] When asked about her first role in Hindi films she said that "[w]hen Shaktida told me that I have to play a blind lady I was taken aback.

[...] When I reached the studio I was excited to see Bollywood luminaries like Nutanji, Dadamoni (Ashok Kumar fondly called), Rajesh Khanna, S. D. Burman and others.

In 1974, she acted with the then-struggling Amitabh Bachchan in the thriller Benaam and opposite Rajesh Khanna in the drama Humshakal.

Her most successful film came at the end of 1974, where she played a rape survivor, in Manoj Kumar's Roti Kapada Aur Makaan.

She went on to become a part of several successful films like Swarag Narak, Maang Bharo Sajna, Pyaasa Sawan, Jyoti Bane Jwala with Jeetendra, Swayamvar with Shashi Kapoor and Anand Ashram with Rakesh Roshan.

She was paired with Vinod Mehra in 10 films,[7] including Anuraag, Us-Paar, Raftaar, Umar Qaid, Mazaaq, Zindagi and Do Jhoot.

In 1982, she did the Marathi film (cameo in song Tumhi Adkitta Mi Ho Supari) Bhannat Bhanu.

Occasionally, she got lead roles in films in the 1990s such as Ghar Parivaar and Aa Ab Laut Chalen, both opposite Rajesh Khanna, then Santaan, Prateeksha (1993) and Udhaar Ki Zindagi with Jeetendra and Keemat: They Are Back (1998).

Apart from Balika Badhu (1967) her Bengali films as lead heroine include Parineeta (1969), Anindita (1972), Anand Ashram (1977), Ogu Bodhu Sundari (1981), Prarthana (1984), Shatarupa (1989), Kari Diye Kinlam (1989), Bidhilipi (1991) and later as supporting actress; Nater Guru (2003), Bhalobasar Anek Naam (2005), The Japanese Wife (2010) and Goynar Baksho (2013).