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.

  • Papers, maps, paintings, drawings, official records and published works related to James Cook and his voyages
  • Around 4,000 books and serials on theosophy, Indian philosophy, comparative religion and related topics. Also correspondence, notebooks, files, etc. on the history of theosophy in Australia, lives of Helena Blavatsky and Krishnamurti, and the Liberal Catholic Church in Sydney
  • 1809 books and serials, published in Australia, Europe and America, relating to gardening, horticulture, botany and agriculture
  • Over 6000 books, pamphlets and journals mainly related to Australian history and politics, but there are also a significant number of British and American imprints. Also personal papers plus 399 subject files of material
  • 696 books and pamphlets relating to freshwater fishing. The majority are British, but also include about 130 Australian works and a number published in New Zealand and America. Most date from the twentieth century, but also include some nineteenth-century imprints.
  •  Papers, photographs, ephemera, aero-philatelic material, objects, books and pamphlets relating to Australian aviation
  • Around 6500 books, 160 serial titles and 918 reprints of individual articles in the subject areas of patristic studies, liturgy, canon law, Biblical studies, church history, biography, cathedrals and other religions
  • About 760 charts, plans and coastal views, most published by Dalrymple between 1769 and 1807, letters to and from Dalrymple and 40 books and pamphlets written or compiled by him between 1767 and 1806, plus 15 other books containing references to him 
  • Papers and oral history recordings conducted by Gwenda Davey on Australian folklore, with an emphasis on children's folklore
  • 1290 recordings of interviews and readings from many of Australia's poets, artists, writers, composers, actors, academics, publishers, librarians, scientists, anthropologists, public servants and some politicians 

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