Léon (1881-1966) and his brother Gustave (1877-1943) studied at the Academy of Fine Arts in Ghent in 1893. First he joined Vie et Lumière, a circle of luminist and impressionist artists, founded in 1904 around Theo van Rysselberghe. In 1905, the brothers joined the second group of Sint-Martens-Latem, the art group that went to live in the region around Sint-Martens-Latem to come into contact with the simplicity of the Leie region to create a new, deeper art. Friendships were formed there with artists Valerius De Saedeleer, Maurice Sys, Constant Permeke, Frits van den Berghe, the brothers Gustave and Karel Van de Woestyne.
Léon became an admirer of Emile Claus and the Luminist School (influenced by Impressionism). Léon De Smet's oeuvre is classified as impressionism and pointillism. His color palette is usually slightly more muted, although a great diversity of colors always arises in his works. His compositions are mainly very balanced.
In 1909 De Smet represented Belgium at the Venice Biennale. In 1910 he took part in an international exhibition in Brussels together with Pierre Bonnard, Édouard Vuillard and James Ensor.
At the beginning of the First World War, Léon fled to Great Britain, where he became a celebrated artist. He had an exhibition at the Leicester Gallery in 1917. The De Smet family settled in the quiet village of Torquay in Devon.
De Smet bleef gedurende de jaren twintig en dertig van de vorige eeuw op grote schaal exposeren in Gent, Antwerpen, Brussel, Parijs, Amsterdam en Pittsburgh. 1930 verhuisde de kunstenaar naar Deurle. In 1953 werd hij geëerd in het Gentse Museum voor Schone Kunsten met een grote, individuele tentoonstelling. Dit Museum heeft nog steeds veel werk van hem; ook Singer heeft enkele werken.