Modot lived in Montmartre at the beginning of the 20th century where he met Picasso and Modigliani.
He played in Germaine Dulac and Louis Delluc's avant-garde films La fête espagnole (1919) and Fièvre (1921).
He had his first role in a sound film with René Clair's Sous les toits de Paris (1930).
He and Jean Gabin are main characters in Julien Duvivier's Pépé le Moko (1937).
He acted in the Jean Renoir classics La grande illusion and La règle du jeu as well as the three-hour poetic film Les enfants du paradis (1945) for Marcel Carné.