Chhaya Devi has acted not only in Bengali films but Hindi, Tamil and Assamese films as well. Till date Chhaya Devi is popular as much as she was in the 1930s. Chhaya Devi has acted in around 150 films. Her family was always associated with the performing arts. In Kolkata she was introduced to Debaki Bose. In Sonar Sansar (1936), directed by Debaki Bose, Chhaya Devi appeared in a lead role for the first time in her career. But it was Bidyapati in 1937 that she got noticed. The film was released in both Hindi and Bengali. This film is considered to be one of the finest films of the New Theatres.

In Bidyapati she portrays the role of Queen Lakshmi who falls in love with the court poet, Bidyapati. The disturbed king dies of shock and the queen drinks poison that is offered to her by the scheming chief minister. This film brought national recognition for her. Early in her career Chhaya Devi often appeared in the films of director Jyotosh Banerjee. Chhabi Biswas was her frequent co star. Some of the notable films in which she acted are Nirjan Saikate (1963) by Tapan Sinha, Hatey Bazarey (1967) and Apanjan (1968). The latter tells the tale of an old woman who takes care of a band of boys who are termed as ruffians. The film was remade in Hindi with Meena Kumari in the lead and Vinod Khanna and Shatrughan Sinha. Chhaya Devi was also part of Mrinal Sen films like Raat Bhore (1956) and Abasheshe (1962).

At a later stage in her career Chhaya Devi shifted to character roles. One of the most memorable roles was in Saat Paake Bandha (1963) where she played the role of Suchitra Sen`s arrogant and authoritarian mother whose over concern about her daughter ruins her marriage. Her other films include Abhinetri (1940), Samadhan (1943), Era Bator Sur (1955) in Assamese, Saptapadi (1961), Uttar Falguni (1963), Arohi (1964), Antony Firingee (1967), Arundathi Devi`s Padi Pishir Barmi Baksha (1972), Pathe Holo Deri and others. Chhaya Devi was also seen Alaap (1977) in Hindi where she steals the show away from Amitabh Bachchan and Rekha.

Chhaya Devi`s demise in 2001 left behind a void in Bengali cinema. Performers like her are rare in the history of Bengali cinema. She has also sung on AIR - All India Radio. The spontaneity and ease with which Chhaya Devi performed established her as one of the most revered Bengali actors in Indian cinema.