Chitra Singh met Jagjit Singh in Mumbai (then known as Bombay), India, in the late 1960s, and they started a musical career together by singing jingles for various advertisements. Their career took off with the launching of The Unforgettables, an album with several firsts to its credit. Their public singing before large audiences revolutionized ghazal singing. Until then, ghazal singing had been confined to musical performances ("mehfils") before small audiences consisting primarily of the elite in the society.
The duo composed and sang songs for Hindi, Punjabi and Bengali albums. They contributed to devotional music by releasing albums which included Krishna, Chirag, Hey Ram, and Shabads. Krishna is one of the largest-selling titles in its category. Chitra has sung popular Bengali songs which are still popular in West Bengal and Bangladesh. "Ki Dile Amai Tumi?" (What have you given me?), "Bujhini To Ami" (I didn't understand), "Duti Mon Ar Nei Dujonar" (Two hearts are one), "Amar Chokher Joler Majhe" (In my tears) are some of her great Bengali songs.
After the death of their son, Vivek, in a car accident in Bombay, Chitra stopped singing and retreated from the limelight. (She has been learning and working on different forms of spirituality, and practices spiritual healing therapies.) Some of Singh's memorable songs include "Yeh Tera Ghar, Yeh Mera Ghar", "Tum Aao To Sahi", "Woh Nahin Milta Mujhe", "Saare Badan Ka Khoon", and "Mitti Da Bawa". Singh's voice is, was and will be for ghazals, producing soulful gems like "Lab-e-Khamosh Se" (album Beyond Time). Her clear, touching and high-pitched voice provided a perfect blend with Jagjit's deep baritone and smooth voice. Their duets created an extraordinary effect in songs like "Ishq Mein Ghairat-e-jazbaat Ne", "Aaye Hain Samjhane Log", and "Uski Hasrat Hai Jise Dile Se Mita Bhi Na Sakoon". Her voice also had a special dimension within the gamut of ghazal singing, so that in the case of "darbari mehfil" ghazals (as in "Dil-e-Nadaan Tujhe", "Dil He To Hai", and "Har Ek Baat Pe Kehteh Ho" from the album, "Mirza Ghalib") she was almost unparalleled.
She had a daughter, Monica (from her previous marriage) who committed suicide in 2009. Jagjit and Chitra's only son Vivek died in an accident in July 1990. Chitra stopped singing after this.