Leela Naidu was born in Bombay (now Mumbai), India. Her father, Dr Pattipati Ramaiah Naidu, a well known nuclear physicist , hailed from Madanapalle, Chittoor Dist., Andhra Pradesh, who had worked under the supervision of Nobel Laureate Marie Curie for his doctoral thesis in Paris, running one of her labs and was Scientific Advisor to UNESCO for Southeast Asia, and later, an advisor to the Tata group. Her mother, journalist and Indologist, Dr. Marthe Mange Naidu, was of Swiss-French origin, from Pont d’Avignon, South-France and earned her Ph.D. from the Sorbonne. She was the only surviving child out of eight pregnancies as Marthe had seven miscarriages. Leela Naidu met Salvador Dali in Grand-hotel Opera, Paris where he painted a portrait of her. Sarojini Naidu, a senior Congress leader and freedom fighter was her aunt. Leela Naidu made her film debut alongside Balraj Sahni in Anuradha (1960), directed by Hrishikesh Mukherjee. Mukherjee cast Naidu in the role after he happened to see one of her pictures taken by Kamaladevi Chattopadhyay. Though it was not successful at the box office, the film went on to win the National Film Award for Best Feature Film, and garnered Naidu critical acclaim. The movie’s music, including the songs Haye re woh din kewn na aaye, Jaane kaise sapnon mein kho gayin ankhiyan and Kaise din beete kaisi beeti raatein, were composed by sitar maestro Ravi Shankar. Naidu’s next film was Nitin Bose’s Ummeed (1962), alongside Ashok Kumar and Joy Mukherjee. She played an offbeat role as an adulterous wife in Yeh Raaste Hain Pyaar Ke (1963), directed by RK Nayyar. The movie, which co-starred Sunil Dutt and Rehman, was based on the real life case K. M. Nanavati vs. State of Maharashtra. Despite its topical nature and controversial theme, the movie flopped; however, some of its songs, notably Ye Khaamoshiyaan, Ye Tanahaaiyaan, became quite popular.

In 1963, Leela Naidu played the lead role of a rebellious young bride in the first Merchant Ivory film, The Householder, directed by James Ivory. According to Leela in her 2009 semi-biography, Ismail Merchant and James Ivory had approached her about making their first ever feature movie with a story about an archaeologist but this fell through as the backers did not like the film script. She then suggested to Merchant-Ivory, making a movie about a book called The Householder by Ruth Prawer Jhabvala which led to their introduction to Ruth and a fruitful lifelong partnership. Satyajit Ray loaned his crew, got many of the actors he used in his movies to act in this movie, selected the music and musicians, and re-cut and reedited the final version, thus guiding and teaching Merchant-Ivory in movie making technique which they successfully used in their award winning movies and documentaries in the future. After watching her performance in the The Householder, Satyajit Ray who had actually assisted and guided Merchant-Ivory in their first film venture, planned an English film, The Journey, with Marlon Brando, Shashi Kapoor and Naidu, but sadly the film was never made. She was considered for the role of Rosie in Vijay Anand’s Guide (1965), but the role required a trained dancer, and so Naidu lost out to Waheeda Rehman. Her last film in Hindi mainstream cinema was Baghi (1964) a costume extravaganza co-starring Pradeep Kumar, Vijaya Choudhury, and Mumtaz.

Later, Leela Naidu made a guest appearance in the Merchant-Ivory film, The Guru (1969). She returned to cinema in 1985 to play a Goan matriarch in Shyam Benegal’s period film, Trikaal. Her appearance in Electric Moon (1992), directed by Pradip Krishen, turned out to be her last cinematic role. She turned down Raj Kapoor four times when he approached her for casting her in his films. In September 2009, Lila, a documentary on Leela Naidu’s life, by Bidisha Roy Das and Priyanjana Dutta was released. Leela Naidu died in Mumbai on 28 July 2009, due to lung failure after a prolonged bout of influenza, at the age of 69.