In 1902 John Le Gay Brereton was selected from ninety-one applicants for the position of Assistant Librarian. He was promoted to Librarian in 1914.

Brereton was responsible for creating a card catalogue and introduced a professional approach to organization and service. By the time of his resignation in 1921 to take up the Chair of English Literature, the staff had increased to 11 including two in a Law Library in the city and the collection exceeded 100,000 volumes. He was succeeded by Henry M Green.

Green guided the Library for a quarter of a century, through the years of the Great Depression, when only the income from the Fisher fund saved the Library from complete stagnation. On his appointment he submitted a report arguing for more staff, salary increases to match those at the Public Library, and "most important of all, there is a whole series of catalogue records where there should be only one".

In 1922 two additional positions were approved and Green appointed the first women as library assistants. Early staff included K W Binns, who became Commonwealth Parliamentary Librarian and J W Metcalfe, who became Principal Librarian, of the Public Library of NSW and a key figure in library development in Australia. An extension to the book stack was commenced in 1924 and ten years later the collection exceeded 200,000 volumes.

By 1935 the staff had grown to 16, including three in Law, and one in the Medical School. When the new Medical School opened in what is now the Blackburn Building in 1935, it included an octagonal Medical Library.

Green was succeeded in 1946 by his Deputy, Edward V Steel, a member of the staff since 1911. The twelve years of Steel's incumbency coincided with an escalation in student numbers, which outpaced the Library's ability to provide adequate resources or services.

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