Zagallo is most renowned for playing a significant role in a record four separate World Cup-winning campaigns for Brazil, including two as a player, one as a manager and one as an assistant coach.
The former forward was also at the 2002 tournament as a special adviser as Brazil won their fifth, and most recent, World Cup.
Zagallo was manager as Brazil reached the final in 1998 too, while he returned for one final World Cup campaign as a technical assistant in 2006.
"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."
"The CBF and Brazilian football mourn the death of one of its legends," added Brazilian Football Confederation (CBF) president Ednaldo Rodrigues.
"The CBF offers solidarity to his family and fans in this moment of sadness at the departure of this idol of our football."
Zagallo's two World Cups as a player came back to back in 1958 and 1962, scoring in the 1958 final as Brazil, inspired by a teenage Pele, were crowned world champions for the first time in Sweden before retaining the title in Chile four years later.
Zagallo was the last surviving member of the team that started the 1958 final, while he was named in the All-Star team for his contributions in 1962, when Brazil's talisman Pele was forced to miss a large chunk of the tournament due to injury.
The Atalaia-born attacker then went on to manage the national team after hanging up his boots, masterminding the 1970 World Cup-winning team that is regarded by many as the greatest side in the history of football.
In doing so, Zagallo became the first person to win the World Cup as both as player and a manager, a feat since emulated by Franz Beckenbauer and Didier Deschamps.
Zagallo remained in charge for the 1974 tournament, when Brazil finished fourth, before serving as assistant to Carlos Alberto Parreira in 1994 for his and Brazil's fourth World Cup title - a tally no other individual can equal.
The legendary figure then returned to take charge of the team in 1998, a tournament which Brazil entered as favourites before being beaten by hosts France in the final, when star striker Ronaldo suffered a mysterious fit on the morning of the match.
Zagallo was also on the pitch as a soldier as Brazil lost the 1950 World Cup final to Uruguay at the Maracana - a result still regarded as one of the darkest days in Brazilian sporting history.
In addition to his 33 caps for Brazil and inextricable links to World Cups, Zagallo represented Flamengo and Botafogo at club level, notably teaming up with his fellow Brazil international winger Garrincha at the latter.
Zagallo went on to manage both clubs multiple times, beginning his coaching career at Botafogo before getting the Brazil job, and going on to spend four different stints in charge of the club, as well as three spells in charge of Flamengo.
At international level, Zagallo took charge of Kuwait, Saudi Arabia and United Arab Emirates during his well-travelled career, steering the latter to a first-ever World Cup in 1990.
In total, he took charge of more than 1,200 games as a manager, while he won 15 domestic titles, a Copa America, a Confederations Cup and an Arabian Gulf Cup throughout his career, in addition to his four World Cups.