Serle was born in Victoria and for many years worked in a life assurance office before becoming chief clerk and accountant at the University of Melbourne. He married artist Dora Beatrice Hake.

He ran a second-hand bookshop during the depression; was guide-lecturer at the National Gallery of Victoria; curator of the Art Museum of the Gallery; and member of the council of the Victorian Artists' Society. He was also president of the Australian Literature Society.

Serle's publications included an edition, with notes, of "A Song to David and Other Poems" by the eighteenth century English poet, Christopher Smart.; "A Bibliography of Australasian Poetry and Verse: Australia and New Zealand"; "An Australasian Anthology" (with 'Furnley Maurice' and R H Croll); "Dictionary of Australian Biography"; and "A Primer of Collecting."

The Dictionary took more than twenty years to complete and contains more than one thousand biographies of prominent Australians or persons closely connected with Australia. Serle comments in the Preface that "I have endeavoured to make the book worthy of its subject. It would have been better could I have spent another five years on it, but at seventy-five years of age one realizes there is a time to make an end."