Her best-known work is the novel By Grand Central Station I Sat Down and Wept (1945), an extended prose poem inspired by her romance with the poet George Barker.Smart was born to a prominent family in Ottawa, Ontario; her father, Russel Smart, was a lawyer, and the family had a summer house on Kingsmere Lake located next door to the future Prime Minister of Canada, William Lyon Mackenzie King.

[3] [page needed] At the age of 11, Smart was confined to bed for a year due to a misdiagnosed "leaky heart valve".

As a result, Smart socialized with many members of Ottawa's political class who were or would become important figures in Canadian history, including acquaintances such as Graham Spry, Charles Ritchie, Lester B. Pearson, and William Lyon Mackenzie King.

[1][3][5] [page needed] At the age of 18, following graduation from secondary school, Smart traveled to England to study music at the University of London.

Barker attempted to visit her in Canada, but Smart's family influenced government officials: he was stopped at the border and turned back because of "moral turpitude".

[3] Just 2000 copies of By Grand Central Station I Sat Down and Wept were published in 1945 by Editions Poetry London, and it did not achieve popularity until its paperback reissue in 1966.

"The power of emotion to transform one's perspective on the world," a recent Open Letters Monthly review of the novel states, "is the theme of this wildly poetic novel.

Christopher Barker writing in The Guardian about this period noted: "On many occasions through the early Sixties, writers and painters such as David Gascoyne, Paddy Kavanagh, Roberts MacBryde and Colquhoun and Paddy Swift [Swift lived downstairs from Smart and his wife, Agnes, wrote cookbooks with Smart] would gather at Westbourne Terrace in Paddington, our family home at that time.

Meanwhile, By Grand Central Station I Sat Down and Wept had been circulating in London and New York, acquiring a cult following that led to its paperback reissue in 1966 and critical acclaim.

Eager to make up for the time away from creative writing forced by the demands of raising her children, Smart wrote voluminously and on a number of subjects, poetry and prose, even her passion for gardening.

In 1977, following a 32-year absence from the book world, Smart published two new works, The Assumption of the Rogues & Rascals and a small collection of poetry, titled A Bonus.

The publication of her journals in On The Side of the Angels brought further posthumous critical appreciation[10][11][12] Morrissey, former lead singer of the British band the Smiths, has talked of his love for Elizabeth Smart.