The former Santos and Corinthians 'keeper had been in poor health for several years since suffering a stroke and died after a heart attack.
Gylmar dos Santos Neves began his career at Jabaquara, a small club in his home town of Santos, but he was there for less than a year before being snapped up by Corinthians.
He played for the Sao Paulo side from 1951-61, winning three Paulista state championships and having the dubious honour of going down in history as the man between the sticks when Pele scored his first professional goal.
Gylmar left Corinthians in 1961 to return home to a team that was emerging asBrazil's pre-eminent club side.
Alongside Pele and other stars such as Coutinho and Pepe, Gylmar helped guide Santos through the greatest period in their history.
During his seven years in goal at the Vila Belmiro, Santos won the Copa Libetadores twice, the World Club Championship twice and five Paulista state championships.
Gylmar played for Brazil on 104 occasions and was on the losing side just 16 times.
His son, Marcelo Neves, was instrumental in forming an association of former World Cup-winning players, campaigning for older players, many of whom were living in undistinguished circumstances, to receive a bonus and monthly pension for their contributions to Brazilian football.
Marcelo's father's death comes just a month after that of Djalma Santos, the full back in the triumphant 1958 and 1962 sides, who passed away aged 84. Another full back in the 1958 team, Nilton De Sordi, died on Saturday, aged 82.