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.

  • About 1750 musical scores comprising general musical arrangements by Flynn, and also both printed and manuscript orchestral and vocal scores, scripts and parts arranged for Radio 3GB 
  • 911 water colours by Adam Forster of Australian flowers, painted between 1916 and 1927.
  • 2457 plays published in France between 1701 and 1840. They include tragedies, comedies, historical dramas, vaudevilles, comic operas and operas.
  • Around 12,000 pamphlets, tracts, reports, addresses and speeches, published in France between 1787 and 1799.
  • Diaries, notebooks, letters, personal papers of the artist Donald Friend and works about Friend.
  • Papers and microfilm of original records relating to the German colonies in the Pacific from 1884-1914, and a selection of other books on this topic.
  • Oral history interviews by Diana Giese with Chinese Australians, Cambodian refugees and community leaders, and with people involved in the Australian publishing industry.
  • Official records, reports and correspondence of the Snowy Mountains Hydro-electric Authority and minutes, agenda papers and correspondence of the Cooma Municipal Council (1956–62) and the Monaro County Council (1957–62). Also around 750 Australian town and district maps. 
  • 95 watercolours and about 80 wash, sepia wash or pencil drawings plus a large number of lithographs and chromolithographs engraved by S.T. Gill, as well as wood engravings, lithographs and photolithographs based on his paintings and sketches.
  • Papers, maps, plans, photographs, paintings and other material related to early Canberra and the work of Walter Burley Griffin and Marion Mahony Griffin.

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