In 1963, Mangeshkar returned to collaboration with S. D. Burman. She also sang for R. D. Burmans very first film Chhote Nawaab and later for his films such as Bhoot Bangla (1965), Pati Patni (1966), Baharon ke Sapne (1967) and Abhilasha (1969). She also recorded several popular songs for S. D. Burman, including Aaj Phir Jeene Ki Tamanna Hai, Gata Rahe Mera Dil (duet with Kishore Kumar) and Piya Tose from Guide (1965), and Hothon Pe Aisi Baat from Jewel Thief (1967).During the 1960s, Lata Mangeshkar continued her association with Madan Mohan which included the songs Aap Ki Nazron Ne Samjha from Anpadh (1962), Lag Ja Gale and Naina Barse Rim Jhim from Woh Kaun Thi? (1964), Woh Chup Rahen To from Jahan Ara (1964), Tu Jahan Jahan Chalega from Mera Saaya (1966) and Teri Aankho Ke Siva from Chirag (1969).
The 1960s also witnessed the beginning of Mangeshkars association with Laxmikant Pyarelal, the music directors for whom she sang the most popular songs in her career. Starting in 1963, Laxmikant Pyarelal association with Lata Mangeshkar grew stronger over the years. Lata Mangeshkar sang over 700 songs for the composer duo over a period of 35 long years, most of which became huge hits. She sang for Parasmani (1963), Mr. X in Bombay (1964), Aaye Din Bahar Ke (1966), Milan (1967), Anita (1967) Shagird (1968), Mere Hamdam Mere Dost (1968), Intaquam (1969), Do Raaste (1969) and Jeene Ki Raah for which she got her 3rd Filmfare Award.
She also sang several playback songs for Marathi films, composed by Marathi music directors including Hridaynath Mangeshkar, Vasant Prabhu, Srinivas Khale, Sudhir Phadke and herself (under the name Anandghan). During the 1960s and 1970s, she also sang several Bengali songs, composed by music directors like Salil Chowdhury and Hemant Kumar. She also made her Kannada debut in 1967 for the film Krantiveera Sangolli Rayanna by recording two songs for the music director Lakshman Berlekar. The song Bellane Belagayithu was received well and appreciated.In this period Lata Mangeshkar has recorded duets with Mukesh, Manna Dey, Mahendra Kapoor, Mohammed Rafi, and Kishore Kumar. For a brief period during the 1960s, she was not on good terms with Mohammed Rafi over the issue of royalty payments to singers. Mangeshkar wanted Rafi to back her in demanding a half share from the five percent song royalty that the films producer conceded to select composers.But Rafi took a diametrically opposite view, and believed that a playback singers claim on the filmmaker ended with the payment of the agreed fee for the song. This led to tensions between the two. After an argument during the recording of the song Tasveer Teri Dil Mein (Maya, 1961), the two refused to sing with each other.The music director Jaikishan later negotiated a reconciliation between the two.