[1] Ayres worked there for eight years; her time there included the development of AustLit, a clearinghouse for information about Australia's literary and print-culture history.

[3] Her position as the Assistant Director-General included managing Trove, a search engine which aggregates resources from cultural institutions across Australia.

[1][3] In March 2017 Ayres succeeded Anne-Marie Schwirtlich as Director-General of the National Library of Australia, being appointed for a five-year term.

[3][4] Her work continues to focus on providing access to the cultural history of Australia and addressing the challenges of preserving born-digital content.

[5] Believing in the importance of the legal deposit system as a way to capture the country's identity, Ayres has presided over the building phase and launch of NED, the National edeposit service whereby publishers submit their digital publications directly via a website to fulfill their legal deposit obligations.