Her first appearance onscreen was the Tamil film Chitthi (1966). Her first film in Malayalam was Poojapushpam (1969), directed by the patriarch Thikkurissy Sukumaran Nair.She ended up being a part of 3 of the 6 movies Thikkurissy directed in his prolific season as a director. She also got to share screen space with the leading lady of the times Sheela in her debut movie itself.

She gained popularity due to her beauty in Malayalam film history. She was a contemporary of the popular Malayalam actress Jayabharathi. Her most notable films are Angathattu (1973), Postmane Kananilla (1972), Lanka Dahanam (1971), Maravil Thirivu Sookshikkuka (1972), Pacha Nottukal (1973), Taxi Car (1972), Aromalunni (1972), Ponnapuram Kotta (1973). In all these films, she starred opposite Prem Nazir and the Prem Nazir-Vijayasree pair created biggest hits in box office. "Theirs was the most successful pair in Malayalam cinema ever,I cannot think of a single film of theirs flopping." says R. Gopalakrishnan, one of the senior-most still photographers in Malayalam cinema. Many of her movies are directed by Kunchacko. At the end of her career she parted ways with Kunchacko and joined with P. Subramaniam. She also acted in a number of Tamil films but in supporting roles. She had played an important role in Babu (1971), a `Sivaji 'Ganesan starrer, as the pair of Sivaji who is killed early in the story. She had also acted opposite Gemini Ganesh in Chitthi, a hit. Other notable ones are Deivamagan (1970), Adhe Kangal (1967) and Kulavilakku (1968).

Many celebrities praised the beauty of Vijayasree. “She is the most beautiful woman I have ever met”, said director Bharathan to his associate, Jayaraj, once. "She was verily the Marilyn Monroe of Malayalam. No other actress had as many male admirers as she had. No other actress had as many hits as her in such a short span of time. No actress had made such a sudden impact in Malayalam cinema. People went to the theatre to see her, and that is something that has not happened before (her time)”, said Jayaraj. He directed a film Naayika,by which the character in the movie named 'Vani' (played by actress Sarayu) portrays slight resemblance to Vijayasree's life." If Jayan epitomised the essence in manly beauty among male actors, then there has never been an actress in Malayalam whose voluptuous beauty compared to Vijayasree’s. Her graceful statuesque beauty was almost a symbol of God’s artistry", said actor Kaduvakulam Antony. Many actors and directors said, due to the bad fate, Malayalam film fans could not see the great Jayan-Vijayasree combination on the screen. “She was extremely beautiful of course, but she was a capable performer too.”, said actor Raghavan.

She committed suicide at the age of 21 on March 17,1974, because of constant blackmailing from Kunchacko, who caught some accidental nude clips of Vijayasree during a bath scene song 'Valliyoor Kaavile' from the movie Ponnapuram Kotta. Kunchacko is the director of that movie. There is also a mention of an interview that Vijayasree had given to Nana Film Weekly in 1973 ( presumably post the month of March 1973, when Ponnapuram Kotta was released) where she lashes out at this certain ‘respectable’ Producer-Director who has ended up being a Monster and her career-nemesis. It is also said that Kunchako (with the support of his brother Navodaya Appachan) murdered Vijayasree. After two years, Kunchako dies on the fifth death anniversary of legendary Malayalam actor Sathyan. Kunchako's Udaya Studios faced heavy losses later.

Vijayasree loved children with all her innocence, she used to distribute sweets or candies whenever she saw children nearby. The videos of Vijayasree on Youtube is still a sensation and visited by many fans including youngsters and aged people.^{[citation needed]}

Malayalam

Tamil

Kannada

Hindi

1. Hum Junglee Hain (1973)

Telugu

1. Manchi Kutumbam (1968)