1957 he was appointed head coach of the national team. Until 1966 and between 1975 and 1978 he led the side through 117 matches. He led Hungary to the World Cups of 1958, 1962, 1966 and 1978. At the Olympics of 1960 in Rome and the 1964 European Nations' Cup the team finished third. The greatest success was the winning of the gold medal at the 1964 Olympics in Tokyo.
His most successful time as club coach was from 1967 and 1971 with Újpesti Dózsa in Budapest, where he laid the beginnings of the club's golden era. The front row consisting of Fazekas – Göröcs – Bene – Dunai II – Zámbó was one of the finest of the 1970s. He took the club to doubles of cup and championship in 1969 and 1970 as well as to a third consecutive championship in 1971, the first titles for the club in a decade. He also took the club to the finals of the Inter-Cities Fairs Cup of 1968/69 against Newcastle United, however losing there 0–3 and 2–3.