The 88-year-old suffered a heart attack on Saturday and had been in an induced coma in Madrid's Gregorio Maranon hospital.
Real Madrid confirmed the news, saying Di Stefano, their honorary president, died at 1715 CET (1615 BST).
A forward, he won five straight European Cups, scoring in each final between 1956 and 1960.
Real president Florentino Perez said he and the club's board would 'like to express deepest condolences and all their love and affection to his children, their families and friends'.
The Argentina-born player also won eight Spanish league titles and was voted European player of the year in 1957 and
1959.
Alfredo Di Stefano's honours
Five European Cups
1956, 1957, 1958, 1959, 1960 (Real Madrid)
Eight Spanish leagues
1954, 1955, 1957, 1958, 1961, 1962, 1963, 1964 (Real Madrid)
One Spanish Cup 1962 (Real Madrid) One
Intercontinental Cup 1960 (Real Madrid)
Two Argentine leagues 1945, 1947 (River Plate)
One America Cup 1947 (River Plate)
Four Colombian leagues 1949, 1951, 1952, 1953 (Millonarios Bogota)
He left Real in 1964 at the age of 38, having scored more than 300 goals across 11 seasons.
Di Stefano played at international level for three nations but never appeared at the World Cup. He won six caps for Argentina and played four times for Colombia during a spell in that country's league. However,
his Colombia caps are not officially recognised by Fifa.
Fifa said in 1954 he could not play for Spain but reversed that decision in 1957 after he gained citizenship and he went on to win 31 caps, scoring 23 goals.
The football world was quick to pay its respects. Manchester United tweeted: "We're sad to hear @realmadrid legend Alfredo Di Stefano has passed away.
The thoughts of everybody at #mufc are with his family & the club."
United's Spanish goalkeeper, Madrid-born David De Gea, added: "A sad day for the world of football. One of the greatest has passed away. RIP Don Alfredo Di Stefano."
Former England striker Gary Lineker wrote: "One of the greatest players ever. Scored in 5 successive European Cup
finals. A feat never to be matched."
Arsenal midfielder Mesut Ozil, who signed for the Gunners from Madrid, tweeted simply: "R.I.P. Alfredo Di Stefano."
Real Madrid confirmed the news, saying Di Stefano, their honorary president, died at 1715 CET (1615 BST).
A forward, he won five straight European Cups, scoring in each final between 1956 and 1960.
Real president Florentino Perez said he and the club's board would 'like to express deepest condolences and all their love and affection to his children, their families and friends'.
The Argentina-born player also won eight Spanish league titles and was voted European player of the year in 1957 and
1959.
Alfredo Di Stefano's honours
Five European Cups
1956, 1957, 1958, 1959, 1960 (Real Madrid)
Eight Spanish leagues
1954, 1955, 1957, 1958, 1961, 1962, 1963, 1964 (Real Madrid)
One Spanish Cup 1962 (Real Madrid) One
Intercontinental Cup 1960 (Real Madrid)
Two Argentine leagues 1945, 1947 (River Plate)
One America Cup 1947 (River Plate)
Four Colombian leagues 1949, 1951, 1952, 1953 (Millonarios Bogota)
He left Real in 1964 at the age of 38, having scored more than 300 goals across 11 seasons.
Di Stefano played at international level for three nations but never appeared at the World Cup. He won six caps for Argentina and played four times for Colombia during a spell in that country's league. However,
his Colombia caps are not officially recognised by Fifa.
Fifa said in 1954 he could not play for Spain but reversed that decision in 1957 after he gained citizenship and he went on to win 31 caps, scoring 23 goals.
The football world was quick to pay its respects. Manchester United tweeted: "We're sad to hear @realmadrid legend Alfredo Di Stefano has passed away.
The thoughts of everybody at #mufc are with his family & the club."
United's Spanish goalkeeper, Madrid-born David De Gea, added: "A sad day for the world of football. One of the greatest has passed away. RIP Don Alfredo Di Stefano."
Former England striker Gary Lineker wrote: "One of the greatest players ever. Scored in 5 successive European Cup
finals. A feat never to be matched."
Arsenal midfielder Mesut Ozil, who signed for the Gunners from Madrid, tweeted simply: "R.I.P. Alfredo Di Stefano."
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