The importance of the establishment of the ANU Library in the development of the university was such that McDonald was appointed by the Interim Council before any of the professors [2].

Initially McDonald and several assistants were housed in Ormond College at the University of Melbourne [3], where they began to form the collection.

ACT schools and incorporated musical groups may borrow orchestral and choral sets for a fee.

[2] In early 2024 the university decided to return most of the collection to the School of Art building once repairs were complete, with frequently used works remaining in the Chifley Library.

Principal subject areas covered include economics, education, fine art, history, languages, linguistics, literature, philosophy, political science, religion, sociology, women's studies and official documents.

On 25 February 2018 all of the books and other items, including precious and rare works, on the lower level were destroyed or damaged by flooding.

In addition, the Menzies Library together with the ANU Archives constitute a major resource centre for Pacific studies.

The Noel Butlin Archives Centre (NBAC)[10] collects business and labour records from Australian companies, trade unions, industry bodies and professional organisations.

The site, and the collection, received considerable public attention after it was featured by the Australian Broadcasting Corporation's station, ABC Local Radio 666AM, in early January 2014, including an online story.

At this time the archives were stored in the upper levels of the Acton Tunnel which passes under the ANU campus.