In 1907 she moved to Paris, taking a job as a correspondent for several Russian newspapers while studying painting under Henri Matisse and attending classes at the Ecole des Beaux-Arts
In 1908 she founded the Académie Russe (Russian Academy) in Montparnasse, renamed the following year as the Académie Vassilieff. The academy was frequented by Chaim Soutine, Amedeo Modigliani, Marc Chagall, Ossip Zadkine, Juan Grisand in 1913 a series of lectures was delivered by Fernand Leger.
Her first works were created under the influence of Cézanne and Matisse. In the 1910s Vasilieva took interest in Cubism (although some researchers believe that back in 1909 she was a follower of “wild and lyrical Cubism”). Georges Braque and Pablo Picasso were her personal friends.
In 1909–1914 Vasilieff travelled extensively around Western Europe, Scandinavia, Romania and Poland. In 1915–1916, despite the war, she visited Russia to participate in the “0.10” exhibition in Petrograd (exhibiting six works), and in the exhibition “Magazine” in Moscow organized by K. Malevich and V. Tatlin. In 1915–1917 she turned her academy into a cafeteria to help painters during the war.
In the 1920s and 1930s, Vasilieff's style of painting changed combining the elements of surrealism and metaphysical school. In 1927, she executed ornamental panels for the Cupola restaurant in Montparnasse (extant). In 1928–1930, solo exhibitions of Vasilieff were held in London and Paris. In 1937, she participated in an international exhibition in Paris, where she created a panel for the Montparnasse rail station.
Marie Vassilieff died at a home for elderly artists in Nogent-sur-Marne, Île-de-France, France, in 1957. In 1998, the Musée du Montparnasse was opened in her former studio.