In 1924, he moved to Paris and began theater studies at the Sorbonne under the guidance of Professor Henri Focillon.
He went on to do research in Armenia, Georgia, Spain, Italy, and Germany, receiving a doctorate from the Sorbonne in 1931.
Between 1933 and 1939 Baltrušaitis taught art history at the Vytautas Magnus University in Kaunas, as well as lecturing at the Sorbonne and at the Warburg Institute in London.
His diplomatic efforts included writing for the French press on Lithuanian issues, and representing Lithuania in international organizations such as the Académie Internationale des Sciences et des Lettres and the Lithuanian Legation in Paris.
Jurgis Baltrušaitis and his wife Hélène Baltrusaitis were family friends of Paul and Julia Child during their residence in Paris in the late 1940s and early 1950s.