He was born, grew up and lived in Adelaide, South Australia, until 1948. His father, a rela-estate developer, proud of his first son, named a street in a new subdivision "Jeffrey": the dogleg street later gave Smart the title of his autobiography, Not Quite Straight.

Smart's first ambition was to be an architect, and the relationship between the constructed environment and people has been a costant theme of his work. From 1939 to 1941, Smart studied at the Adelaide Teacher's College and the South Australian School of Art and Crafts. Literature and classical music were also integral to Smart's aestetic development.

At this time smart also acknowledged his homosexuality, although in conservative Adelaide he had to tread carefully. For five years from 1942, Smart taught art in schools for the South Australian Education Department.

In 1949 he traveled to the US, then to Britain and Europe. After living and studying in Paris, Smart spent a year with artist friends, including Donald Friend, in Ischia on the Bay of Naples before eturning to Australia to live in Sydney.

Smart felt constrined in his private life while he was employed in "The Children's Hour" for Australian Broadcasting Commission, but he and Donald Friend occasionally sought out like-minded men in the "camp" quarters of Sydney.

In 1963 he returned to Italy, where he has lived ever since. At his home in Arezzo some order and stability was established in 1976 when Ermes de Zan moved in. he was not only an assistant to help with painting, but he reorganised the garden, attended to practical matters and provided Smart with emotional support. Their relationship continues.