At her nursing home in Toulon, France, Ms. Randon, who adopted the name Sister André when she enrolled in holy orders in 1944, passed away peacefully.
She was born in southern France in 1904, survived both World Wars, and devoted a large portion of her life to Catholicism.
She informed reporters that "only the good Lord knows" the key to her long life.
Sister André has witnessed 27 French heads of state and was born when the Tour de France had only been staged once.
She passed away on Tuesday, according to David Tavella, a spokesman for her care home.
"There is a lot of sadness, but she wanted to go with her dear brother. It's a liberty for her, "added Mr. Tavella.
It was stated that Sister André and her brothers got along well. When World War One came to a close, she famously told reporters that one of her favourite recollections was of their safe return.
It was unusual, she remembered. Families typically had two dead people rather than two living people.
Sister André cared for other elderly people despite being blind and depending on a wheelchair, some of whom were considerably younger than herself.
Sister André stated: "People say that work kills, but me it saved me life. I remained working until I was 108." in an interview with the AFP news agency in April of last year.
She claimed in the same interview that she would be happier in heaven, while continuing to partake in daily rituals like eating chocolate and drinking wine.
She had held the title of oldest person in Europe for some time when Kane Tanaka, a Japanese woman who lived to be 119 years old, passed away in April of last year, making her the oldest person in the world.
She had previously made the record books. She overcame Covid-19 in 2021 and was the oldest person to do it.
Sister André was baptised at the age of 26 after converting to Catholicism after being raised in a Protestant family.
About 15 years after making the decision to join the Catholic Church, she joined a nunnery known as the Daughters of Charity, motivated by her desire to "go further."
She was given a job at a hospital in Vichy, where she worked for almost 31 years.
She told reporters these things in one of her last interviews: "Instead of hating one another, people should support and care for one another. Things would be a lot better if we shared that information."