In 1959, he launched his career as a professor at the "Julio de Mesquita Filbo" São Paulo State University.
During this time, he oversaw the Unit of Education and Research within the Department of Scientific Affairs of the Organization of American States (OAS).
[2] Returning to Brazil in 1970, Gurgulino de Souza assisted in establishing the Federal University of São Carlos in Sao Paulo and was subsequently named the institution's first Rector.
During the 1970s and early 1980s, he held numerous positions within the Brazilian Ministry of Education and Culture and the National Council for Scientific and Technological Development of Brazil.
Gurgulino de Souza served as Special Advisor to the Director-General of UNESCO from 1997 to 1999 before being elected vice-president of the International Association of University Presidents (IAUP) for the period 1999–2002.