He published some of his own work in limited edition books such as Old Sydney (1911) and Old Colonial By-Ways (1928), prompted by his passion for preserving historic buildings.

[4] He studied pencil and ink drawing at the Julian Ashton Art School (1902–07) and then learnt the techniques of etching from Eirene Mort.

In 1916 he founded a syndicate with Bertram Stevens and Charles Lloyd Jones to publish Art in Australia,[8] and in the same year he founded the commercial art studio and advertising firm Smith and Julius with Harry Julius, specialising in high quality artwork for prestigious clients such as Dunlop[9][10] and Berlei.

[11][12] They employed such prominent Sydney artists as James Muir Auld, Fred Britton, Frank Burdett, Harold Cazneaux, Albert Collins (who was a director from 1916–51), Roy de Maistre, Adrian Feint, George Frederick Lawrence, Percival Leason, John Passmore, Lloyd Rees, Bill Sparrow and Roland Wakelin.

He edited books on J. J. Hilder, Arthur Streeton, Blamire Young, Hans Heysen, Norman Lindsay, Elioth Gruner, Margaret Preston, George Lambert, Douglas Annand, Francis Lymburner and William Dobell.

[19] Sydney Ure Smith led a furiously active public life: he was a foundation member (with Gayfield Shaw, Lionel Lindsay, John Shirlow, Eirene Mort, David Barker, Albert Henry Fullwood, John Barclay Godson, and Bruce Robertson) of the Australian Painter-Etchers Society in 1920 and almost certainly was instrumental in founding its daughter organisation, the Australian Print Collectors' Club in 1925.

He was a trustee of the Art Gallery of New South Wales 1927–47 (and vice-president 1943–47, supporting the controversial 1943 Archibald Prize going to William Dobell for his portrait of Joshua Smith).

An accomplished mimic and raconteur, "on Sunday mornings he entertained a stream of visitors from Europe as well as such friends as Lionel Lindsay, Hardy Wilson and (Sir) Robert Menzies".