As an amateur he won an Olympic gold medal in the road race and the world title in the individual pursuit on track, both in 1956.

[1] Next year he turned professional, and in 1958 won the world title in the road race and the Giro d'Italia.

His best year was 1956, in which he won a gold medal in the road race at the Summer Olympics in Melbourne, and, in September, stripped Jacques Anquetil of the hour record, riding 46.394 km at the Velodromo Vigorelli in Milan.

[1] In 1957 he became professional and won six important races, including the Trofeo Baracchi alongside Fausto Coppi, and became Italian champion.

In 1958 Baldini won the Giro d'Italia,[1] beating Charly Gaul on the latter's favourite terrain, climbing.