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Born in Ukraine, Orloff emigrated with her family at the age of eighteen to Ottoman Palestine (present day Israel) and settled in Jaffa, where she found a job as a cutter and seamstress and joined the left-wing Zionist workers movement Hapoel Hatzair.
After five years in Palestine, Orloff went to Paris - initially to study fashion – and enrolled in sculpture classes at the Académie Russe in Montparnasse. In 1916 she married Polish-Jewish poet Ary Justman (who died during the flue-epidemic of 1919) with whom she had a son, and with whom she collaborated on a book featuring his poetry and her sculpture. Orloff became friendly with other young Jewish artists in Paris at this time; among them Marc Chagall, Jacques Lipchitz, Amedeo Modigliani, Jules Pascin and Ossip Zadkine.
Although her preferred medium was wood, Orloff also enjoyed working in stone, marble, bronze and cement. A sculptor of natural subjects including women as mothers, Orloff is perhaps best known for her sculptured portraits of famous contemporary sitters – Picasso, Matisse and Modigliani for example. In 1913 Orloff exhibited in the Salon d'Automne in Paris that helped establish her critical reputation. Later exhibitions included showings at Tel Aviv Museum (1935, 1949), the Steimatsky Gallery in Jerusalem (1935) and the Petit Palais in Paris (1937).
When the Nazis invaded Paris, Orloff fled to Switzerland with her son and the Jewish painter Georges Kars. In February 1945, Kars committed suicide in Geneva, encouraging Orloff and her son to travel to the United States where they stayed for three years. Returning to Paris in 1948, Orloff discovered her house had been ransacked and the sculptures in her studio destroyed during the years of Nazi occupation. During the 1950s however she produced an impressive series of monumental public sculptures for the new State of Israel. Here Orloff died in 1968 during preparations for a retrospective of her work at the Tel Aviv Museum.