Lydia, his wife of 64 years, was at his side, the Heston family said in a statement.
"Charlton had made an announcement of his Alzheimer's diagnosis in 2002 and had very much retired from public life," a family spokesperson tells PEOPLE. "He had been at home most of the past years."
Heston won the Academy Award for best actor in 1959's Ben-Hur. He also played Moses in The Ten Commandments in 1956. Later in life, he was known as much for his political work than acting, serving as president of the National Rifle Association.
Dick Van Patten, a longtime friend and his costar in the 1973 movie Soylent Green, remembers Heston as a star who "was so nice to everyone" on set – and as an ideal tennis partner. "He was a real gentleman on the court," Van Patten told PEOPLE. "He was an intellectual. He used to read a lot. He was just a nice man. I feel very very bad about it. I'm going to miss him very very much."
Heston's family also paid tribute to the actor in a statement. "Charlton Heston was seen by the world as larger than life," said the statement. "He was known for his chiseled jaw, broad shoulders and resonating voice, and, of course, for the roles he played. Indeed, he committed himself to every role with passion, and pursued every cause with unmatched enthusiasm and integrity.
"We knew him as an adoring husband, a kind and devoted father, and a gentle grandfather, with an infectious sense of humor. He served these far greater roles with tremendous faith, courage and dignity. He loved deeply, and he was deeply loved.
"No one could ask for a fuller life than his. No man could have given more to his family, to his profession, and to his country. In his own words: 'I have lived such a wonderful life! I've lived enough for two people.'"
Reporting by ELAINE ARADILLAS and PAMELA WARRICK
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