Jaywant was born in Bombay (now Mumbai) in 1926. She was first cousin of actress Shobhna Samarth, the mother of actresses Nutan and Tanuja. Since 1983, she had been living mostly a reclusive life.

She was married to director Virendra Desai in the 1940s. Later, she married her second husband, actor Prabhu Dayal, with whom she acted in several movies.^[3]

Nalini Jaywant died on 20 December 2010, aged 84, at her bungalow of 60 years at Union Park, Chembur, Mumbai, India.

In her teens, she appeared in Mehboob Khan's Bahen (1941), a film about a brother's obsessive love for his sister. She performed in a few more movies before filming Anokha Pyaar (1948). In 1950, she garnered fame when she became a top star with her performances opposite Ashok Kumar in Samadhi and Sangram. Samadhi was a patriotic drama concerning Subhas Chandra Bose and the Indian National Army. Although the leading movie magazine of the day, Film India, called it "politically obsolete", it enjoyed success at the box office. Sangram was a crime drama in which Nalini played the heroine reforming the anti-hero. She and Ashok Kumar performed together in other films, such as Jalpari (1952), Kafila (1952), Nau Bahar (1952), Saloni (1952), Lakeeren (1954), Naaz (1954), Mr. X (1957), Sheroo (1957) and Toofan Mein Pyar Kahan (1963).

Nalini remained an important leading actress through the mid-1950s, appearing in such films as Rahi (1953), Shikast (1953), Railway Platform (1955)), Nastik (1954), Munimji (1955), and Hum Sab Chor Hain (1956). The 1958 film Kala Pani, directed by Raj Khosla, was Nalini's last successful movie, for which she won the Filmfare Best Supporting Actress Award. Bombay Race Course (1965) was the last film she made before retirement. After 18 years, she returned as a character actress in Nastik which marked her last film appearance.

• Nastik (1983)
• Bandish (1980)
• Bombay Race Course (1965)
• Toofaan Mein Pyar Kahan (1963)
• Girls Hostel (1963)
• Zindagi Aur Hum (1962)
• Senapati (1961)
• Amar Rahe Yeh Pyar (1961)
• Mukti (1960)
• Maa Ke Aansu(1959)
• Kala Pani (1958)
• Milan (1958)
• Sheroo (1957)
• Mr. X (1957)
• Neelmani (1957)
• Miss Bombay (1957)
• Kitna Badal Gaya Insaan (1957)
• Hum Sab Chor Hain (1956)
• Durgesh Nandini (1956)
• Awaaz (1956)
• Insaaf (1956)
• Fifty Fifty (1956)
• Aan Baan (1956)
• 26 January 1950 (1956)
• Railway Platform (1955)
• Munimji (1955)
• Rajkanya (1955)
• Chingari (1955)
• Nastik (1954)
• Kavi (1954)
• Baap Beti (1954)
• Naaz (1954)
• Lakirein (1954)
• Mehbooba (1954)
• Shikast (1953)
• Rahi (1952)
• Jalpari (1952)
• Saloni (1952)
• Kafila (1952)
• Naubahaar (1952)
• Do Raah (1952)
• Naujawan (1951)
• Jadoo (1951)
• Ek Nazar (1951)
• Nandkishor (1951)
• Sangram (1950)
• Samadhi (1950)
• Muqaddar (1950)
• Aankhen (1950)
• Anokha Pyaar (1948)
• Gunjan (1948)
• Phir Bhi Apna Hai (1946)
• Adaab Arz (1943)
• Aankh Michauli (1942)
• Radhika (1941)
• Nirdosh (1941)
• Bahen (1941)