At the age of 5, Vyjayanthimala got the rare chance of performing a dance before the Pope. At age 15, she got a break in AVM Productions Tamil movie, "Vazhkai", which was directed by M. V. Raman, a family friend. The movie was a success, and was remade in Hindi as "Bahaar" (1951). She acted in a few more Tamil movies before moving on to a highly successful career in Hindi movies. Her dance competition with Padmini in the Tamil film, "Vanjikottai Vaaliban", received much acclaim.

Vyjayanthimala got her initial Hindi movie roles in "Ladki" and "Nagin" (1954). Hemant कुमार's music and her dance accompanying the song, "Man Dole, Mera tan dole", in "Nagin" made the movie an enormous success, and the movie's success helped Vyjayanthimala break out of B grade movies. Bimal Roy cast her as "Chandramukhi" opposite Dilip कुमार in the critically acclaimed "Devdas". She subsequently starred in four successful films opposite Dilip कुमार: "Madhumati", "Ganga Jamuna", "Leader", and "Naya Daur". The first two of those four roles earned her Filmfare Best Actress Awards. She also received a Filmfare nomination as Best Actress for portraying in "Sadhna"' a tawaif (a courtesan) who eventually got rehabilitated in the society. She costarred with Raj Kapoor in "Sangam" which earned her the Filmfare Best Actress Award. (She denied rumors of an affair with Raj Kapoor during the production of "Sangam", saying that it was a publicity stunt by Kapoor to boost his image.)

Vyjayanthimala starred in the 1966 historical epic, "Amrapali", based on the life of the legendary Buddhist courtesan Amrapali. The movie was not a commercial success, and the commercial failure much disappointed her as she considered it the magnum opus of her career. Later, she said that she would like to see a remake of that movie, with Madhuri Dixit playing her role.

She costarred with Dev Anand in "Jewel Thief", with Rajendra कुमार in "Suraj", with Shammi Kapoor in "Prince", and with Kishore कुमार in his inane yet zany comedies,including the blockbuster "New Delhi". Vyjayanthimala's Tamil movies included Vanjikottai Valiban, Irumbuthirai, Then Nilavu, Vaazhkai, Penn, Parthiban Kanavu (old), and Baghdad Thirudan.

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