Cartier-Bresson, whose striking photographs of the death of Indian independence leader Mahatma Gandhi are a key part of his photographic legacy, also spent time documenting the ashram of guru Sri Aurobindo in 1950.
"It's unlike anything from Cartier-Bresson you've seen because it's a bit of an experimental album and an album he possibly didn't want to show people," the curator of the exhibition in New Delhi, Rahaab Allana, told AFP.
A pioneer in the art of photojournalism, Cartier-Bresson combined an eye for design and proportion with a sense of history and the humorous. He died in 2004 aged 95.
Aurobindo was a one-time leader of political resistance to British rule in colonial times who dedicated the latter part of his life to spirituality and yoga at his retreat in the former French colony of Pondicherry.
At the invitation of Aurobindo and his partner, known as The Mother, Cartier-Bresson visited and took rare pictures of the couple together, documenting their life in the beach-side town on India's south-east coast.
When the pictures were published by the Magnum agency, however, an accompanying article was thought to have upset The Mother, who objected to the description of Aurobindo who died shortly after Cartier-Bresson's visit.
"When the material was publicised in Europe, the ashram received a certain amount of bad publicity," Allana explained, adding that there was a sarcastic reference to Aurobindo's self-proclaimed sense of divinity.
As a result, The Mother bought the negatives to the photographs for 3,000 dollars, printed 50 albums for the personal use of people connected with the ashram and thereafter kept the pictures from public sight.
This piece of Cartier-Bresson and 20th-century photographic history might have been lost but for the intervention of Delhi-based art collector Ebrahim Alkazi, the founder of the Alkazi Foundation for the Arts.
He bought one of the printed albums when it came up for auction in London and set about trying to convince the Aurobindo ashram and the Cartier-Bresson Foundation in Paris to agree to an exhibition.
Both eventually consented, leading to the show which will open at the French cultural institute Alliance Francaise in the capital on Saturday and will travel to Pondicherry later in the year.
A total of 118 images from the Cartier-Bresson album, as well as hand-written notes on the project, will be displayed alongside other photographs from artists based in Pondicherry.
The previously unexhibited work "reveals the man and his practice as a whole, not his major edited-down photos which we've seen and we know," added Allana. "They are very different."
Travelling the world with his trusted Leica camera, Cartier-Bresson captured the birth of Communism in China and the liberation of Paris in 1944 "prowling the streets... determined to trap life, to preserve life in the act of living" as he put it.
The Mother, born as Mirra Alfassa in Paris, went on in the 1960s to found Auroville, an experimental township near Pondicherry that incorporates Aurobindo's teachings on human unity and spirituality.