Her father was Maharaja Jitendra Narayan of Cooch Behar in West Bengal, and her mother was the Maratha Princess, Indira Raje of Baroda, the only daughter of Maharaja Sayajirao Gaekwad III, and she was sister to Jagaddipendra Narayan, informally known as 'Bhaiya', who succeeded their father to the throne of Cooch Behar.

After her departure from politics, she lived a quiet life in her large estate, spending time on hobbies and leisure.

She was related to Keshub Chandra Sen (A prominent figure in the Bengal Renaissance and social reformer) through her paternal grandmother, Suniti Devi, who was the daughter of Keshub Chandra Sen.[6][9][10] Her mother was Maratha Princess Indira Raje of Baroda, the only daughter of Maratha King, Maharaja Sayajirao Gaekwad III, an extremely beautiful princess and a legendary socialite.

Gayatri had one child, Prince Jagat Singh of Jaipur, late Raja of Isarda, born on 15 October 1949, who was granted his uncle's fief as a subsidiary title.

[16][17] In a 2004 interview, Gayatri mentioned "I have never felt beautiful...I remember as a young girl, my mother had to literally force me into applying lipstick, physical appearance doesn't bother me, it never has, it never will".

[20] In 2013 designer Sabyasachi made five limited edition saris presented at the Taj Mahal Palace in honour of Devi's enduring style icon status.

[24] Gayatri Devi ran for Parliament in 1962 and won the constituency in the Lok Sabha, winning 192,909 votes out of 246,516 cast.

[25] She continued to hold this seat in 1967 and 1971 as a member of the Swatantra Party founded by C. Rajagopalachari,[12] running against the Indian National Congress.

Despite the fact that her husband was being made ambassador to Spain, she stuck to her principles and decided not to join the party.

Gayatri was arrested under the COFEPOSA Act during the Emergency in July 1975 on the accusation of violating tax laws, and served 5 and a half months in Tihar Jail.

There were rumours that she might re-enter politics as late as 1999, when the Cooch Behar Trinamool Congress nominated her as their candidate for the Lok Sabha elections, but she did not respond to the offer.

She was herself not from the Rajput community, but from a dynasty native to Cooch Behar in Bengal, and was daughter of Maharaja Jitendra Narayan and Maharani Indira Raje, who was daughter of Maharaja Sayajirao Gaekwad III and Maharani Chimnabai, belonging to the Gaekwad dynasty of the Marathas.

Her paternal grandparents were Nripendra Narayan Bhup Bahadur and Sunity Devi of Cooch Behar.