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.