In his first period with Benfica, the club was transformed to professional standards. Otto Glória founded a home for the players and focused on recruiting players from the periphery of the Portuguese capital and also from the African overseas provinces. In these years between 1954 and 1959 the club won two Portuguese championships and three cups.
In February 1962 he takes on the reins with Olympique Marseille. The club was then stuck in the second division and saw its aspirations to return to the first division endangered. In his four months with the club did not lose a single match and achieved its objective.
In his second tenure with Benfica he had continuous success on the national level, winning two more championships and cups. He also led the club into the 1968 final of the European Cup of Champions in London against Manchester United, which was lost 1-4.
At the 1966 FIFA World Cup in England he led the Portuguese national football team, with Eusébio, who became the tournament's top scorer, to the third place. In the process Portugal inflicted a 1-3 defeat on Glória's home country Brazil. The official head coach of the Portuguese team was then Manuel da Luz Afonso.
In 1979 he became with CR Vasco da Gama of Rio de Janeiro runner-up in the Brazilian championship, losing in the final 1-2 against SC Internacional Porto Alegre, which remained undefeated throughout the competition.
In the year thereafter he guided Nigeria through the 1980 African Nations Cup, which the team won in the final in Lagos with 3-0 against Algeria. He left this position after poor performances at the 1982 campaign in Libya.
He went to coach Portugal National Team, in 1982, for the Euro 1984 qualifyings, but he resigned after a 0-4 defeat in a friendly match with Brazil, the following year.