The functions of the Library are set out in section 6 of the National Library Act 1960. They are:

• to maintain and develop a national collection of library material, including a comprehensive collection of library material relating to Australia and the Australian people;
• to make library material in the national collection available to such persons and institutions, and in such manner and subject to such conditions, as the Council determines with a view to the most advantageous use of that collection in the national interest;
• to make available such other services in relation to library matters and library material (including bibliographical services) as the Council thinks fit, and, in particular, services for the purposes of:
  • the library of the Parliament
  • the authorities of the Commonwealth
  • the Territories
  • the Agencies (within the meaning of the Public Service Act 1999); and
• to cooperate in library matters (including the advancement of library science) with authorities or persons, whether in Australia or elsewhere, concerned with library matters.

The Library is one of many agencies in the Communications and the Arts portfolio with responsibilities for collecting Australian cultural heritage materials and making them available to the Australian public. Senator the Hon. Mitch Fifield had responsibility for the Library until 28 May 2019. The Hon. Paul Fletcher MP, appointed Minister for Communications, Cyber Safety and the Arts on 29 May, is the minister responsible for the Library.

The affairs of the Library are conducted by the Library Council, with the Director-General as executive officer.