The actor, musician, activist and member of the stolen generation suffered a stroke and died at Royal Melbourne Hospital on Tuesday, aged 79.
"We're heartbroken to be announcing the passing of our much loved Yorta Yorta senior elder. Uncle Jack Charles," his family said in a statement.
"We are so proud of everything he has achieved in his remarkable life."
Before he passed away, his family were able to send him off on country during a smoking ceremony at the hospital.
The Boon Wurrung, Dja Dja Wurrung, Woiwurrung and Yorta Yorta man's career spanned decades.
While revered as the grandfather of Indigenous theatre, Charles became better known to audiences for his film roles in The Chant of Jimmie Blacksmith (1978) and Blackfellas (1993).
More recently he voiced the frilled-neck lizard character Greg in animated film Back to the Outback (2021).
His works include touring his one-man show Jack Charles v The Crown based on his life, and the ABC TV series Cleverman and Preppers. He also appeared on SBS series Who Do You Think You Are.
Earlier this year, he spoke at Victoria's truth-telling Yoorrook Justice Commission about being a member of the stolen generations, taken from his mother as a four-month-old.
He grew up in the Salvation Army Boys' Home in Box Hill, Victoria and was the only registered Aboriginal child at the home.
Charles said he was taunted because of the colour of his skin.
"I wasn't even told I was Aboriginal - I had to discover that for myself," he told the inquiry.
Prime Minister Anthony Albanese said despite enduring many hardships, Charles uplifted our nation with his heart and his genius, creativity and passion.
"He endured cruelty, he knew pain. He survived every turn of the vicious cycle, holding on to his humanity," he said.
The First Peoples' Assembly of Victoria said there was much heartache across the community following his death.
"They couldn't keep him down, he persisted against all the odds overcoming every challenge thrown his way. All the while radiating joy, passion and love," First People's Assembly of Victoria Co-Chair Marcus Stewart said.
Indigenous Victorian senator Lidia Torpe tweeted: "We've lost our king".
Indigenous rapper Adam Briggs tweeted: "Uncle Jack & Uncle Arch gonna be in good company wherever they're at", referring to Indigenous singer Archie Roach who died in July.
Director Jacob Harris, who worked with Uncle Jack on two occasions, said Australia had lost an "amazing storyteller".
Premier Daniel Andrews, who met Charles on a number of occasions, described him as a great Victorian.
"(He was) someone who took his own personal pain and the great trauma that he'd suffered in his life to be a beacon for others and to campaign for justice," Mr Andrews said.
"It's a very sad day."
The premier said his department would be in contact with Charles' family to "see how best we can celebrate his life".
Federal Minister for Indigenous Australians Linda Burney said Charles was a groundbreaking storyteller and activist who brought people in with his warmth and grace, never shying away from his past and who he was.
"Uncle Jack offered a window for many Australians to see the enduring pain of survivors of the Stolen Generations and inspired people with his strength of character and resilience," she said in a statement.
Former Prime Minister Kevin Rudd also paid tribute, describing Charles as an "enduring figure in arts, culture and in our Australian story".
A portrait of Charles by comedian and author Anh Doh won the People's Choice award at the 2017 Archibald Prize in NSW.
His family have given their permission to use his name and images.
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