Rose, who won the Australian Open and French Open along with five Grand Slam doubles titles, was 87.
"The tennis family is mourning the passing of seven-time Grand Slam champion Mervyn Rose and our thoughts are with his family and friends," said Tennis Australia.
Rose claimed his first major title at the 1954 Australian Open, defeating defending champion and top seed Ken Rosewall on the way to the final, where he beat his long-time doubles partner Rex Hartwig.
Rose was also part of Australia's 1951 and 1957 Davis Cup-winning teams, reaching a career-high three in the world.
After retiring from playing, he made the transition to coaching, working with some of the greats including Court, King and Arantxa Sanchez-Vicario.
He was inducted into the International Tennis Hall of Fame in 2001, the Australian Tennis Hall of Fame a year later and was awarded the Member of the Order of Australia for his service to tennis in 2006.