After his retirement as a player, he became a successful coach, leading the
Brazil national team to its second FIFA World Cup in (
1962). In the first match against
Mexico national team,
Pelé assisted on the first goal and scored the second one, later injuring himself while attempting a long-range shot against
Czechoslovakia national team. This kept him out of the remainder of the tournament and forced Moreira to make his only lineup change of the tournament; bringing in
Amarildo. The replacement duly scored in the
final, a rematch against Czechoslovakia.
Garrincha starred in the 3–1 win.
Moreira managed Brazil national team for 61 matches, with 37 wins, 9 draws and 15 losses. Besides winning the World Cup, he led the "Canarinha" to win the
Taça Oswaldo Cruz in 1961 and 1962,
Taça Bernardo O'Higgins in 1961 and 1966,
Roca Cup in 1963 and
Taça Rio Branco in 1967.