Zagallo was a winger in the Brazil team who won back-to-back World Cups in 1958 and 1962, starting in both finals.
He managed the side widely regarded as the greatest international team of all time, including Pele, Jairzinho and Carlos Alberto, to glory in 1970.
Zagallo’s final World Cup triumph came as Carlos Alberto Parreira’s assistant coach in 1994.
He returned as Brazil manager after that tournament and led them to the final in 1998, where they were beaten by hosts France.
Zagallo was the first person to win the World Cup as both a player and a manager – a feat that has since been matched by Germany’s Franz Beckenbauer and France’s Didier Deschamps.
“With enormous sadness, we inform you of the death of our eternal four-time world champion Mario Jorge Lobo Zagallo,” a statement on his official Instagram account said.
“A devoted father, loving grandfather, caring father-in-law, faithful friend, victorious professional and a great human being. Giant idol. A patriot who leaves us a legacy of great achievements.”
Brazil are the most successful nation in World Cups, with five titles, and Zagallo is one of the most instrumental figures in that history.
As a teenager on national service he was one of nearly 200,000 in the Maracana Stadium who saw hosts Brazil stunned by Uruguay in the decisive final match of the 1950 World Cup.
Speaking to BBC Sport in 2013, Zagallo said: “That day has never left my mind.”
The tactically astute Zagallo, nicknamed ‘The Professor’ and ‘Old Wolf’, pulled together a side filled with the attacking talents of Pele, Jairzinho, Gerson, Tostao and Rivellino and made them irresistible.
Brazil won all six of their games in the 1970 World Cup and swept to a 4-1 victory over Italy in the final.