Aurousseau was the son of George Hippolyte Aurousseau (1864 - 1953), an artist, teacher, and jeweller, who exhibited his work at the Colonial and Indian Exhibition in London in 1886 and the Adelaide Jubilee International Exhibition in 1887, as well as publishing several articles on freehand drawing, and Kathleen Aurousseau, a painter who exhibited her works at the Australian Exhibition of Women's Work in 1907.
He began work at the Australian Museum as an office boy, before undertaking studies in geology and chemistry, graduating from the University of Sydney with a BSc. in 1914. (He was later awarded an honorary D.Litt. from the University of Newcastle, New South Wales.) During World War I, Aurousseau served in France as a captain in the 51st Battalion, for which service he was mentioned in despatches and awarded both the Military Cross and the French Croix de Guerre.
After the war, he returned to Australia and undertook work with the University of Western Australia. He moved to the United States to work for the Geophysical Laboratory, but returned to Australia at the beginning of the Depression. In the 1930s, he moved to Europe to write. During World War II, he was living and working in London.