The National Library's collections range in date from the eleventh century to the present, take in every country in the world and are exceptionally broad in format and subject. They consist of books, pamphlets, periodicals, newspapers, ephemera, maps, manuscripts, private archives, music scores, pictures, microform and digital materials.

A significant proportion of what the Library holds, including some of the rarest and most valuable material, was acquired as collections. Some were built up by individual collectors, families, booksellers and learned societies, often over a long period (formed collections). Other collections have been assembled from various sources by the Library itself in an effort to achieve great strength in particular subject areas (subject collections). Many of the collections have outstanding research value.

The following entries are for the most significant of these collections. The entries give details about the individuals, families or organisations that assembled the collections, describe the size, scope and strengths of each collection, and summarise how they have been acquired, organised, catalogued or listed by the Library. While the majority of the collections described consist largely of Australian materials, there are also entries for significant Asian, European and North American collections. These descriptions are intended to complement the Library's catalogue and other finding-aids.

Between 1974 and 1982 the Library published the Guide to the collections, edited by C.A. Burmester. A number of the collections recorded in that publication have been updated and are included in the following selection.

  • Overseas and Australian sheet music, including some manuscripts, with the main strengths popular songs and piano music of the nineteenth and early twentieth centuries. Also some programs and papers collected by Kathleen Brady 
  • Family papers, maps of the Hong Kong and Macau region, pictures, photographs and a large collection of books and pamphlets predominantly historical works, particularly histories of Portugal, the Portuguese colonies, China and Japan 
  • Around 10,800 items from the period 1829-1922 ranging from a single page to hundreds of pages and documenting British reactions to particular events, problems and crises, as well as Britain's relations generally with particular countries and regions
  • Over 3,000 printed pamphlets, leaflets and issues of periodicals, mostly published 1900-1970 plus a collection of microfiche and microfilm of other publications produced by left-wing parties and organisations in the period 1961–88
  • Small collection of books, pamphlets and serials on race and class relations, migration, urbanisation and other aspects of contemporary society in the Caribbean and Latin America collected by Leonard Broom
  • Photographs and papers, memorabilia and books relating to railways collected by John Buckland
  • Papers, photographs from Europe, Asia, America and Australia ranging from 1850-1950. Also books, journals, booklets, exhibition catalogues on the history of photography or containing illustrations of particular interest collected by Eric Keast Burke
  • Photographs of Australian steamships, nine paintings and an unpublished manuscript 'Dictionary of Australian steamships' by Terence Callen
  • Papers related to Clyde Cameron's long political career, and 12 oral history recordings conducted by Cameron with other political figures
  • Books and pamphlets relating to Portuguese colonies in Africa and Asia, mostly published in Portugal or the colonies from 1840-1950

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