The Library holds original manuscripts and drawings by Australian landscape architects and gardeners, as well as an extensive collection of books, periodicals and articles that deal with Australian and international landscape design and gardening. There is information and source material relating to the layout and design of gardens, dating back to the early colonial period.

Of note is the work of William Guilfoyle, who laid out the grounds in front of the Library in 1875. The photographic documentation of Guilfoyle's gardens at Turkeith and Mooleric in Birregurra, Victoria, was recently commissioned by the Library.

The Pictures Collection and Australian Manuscripts hold a vast amount of material relating to the creative and professional output of Australian landscape architects and designers. Major garden designers whose archives are held include Edna Walling, Ellis Stones, Mervyn Davis, Gordon Ford, John Stevens, Peter Glass, Glen Wilson and Millie Gibson.

The papers of the landscape contractor Eric Hammond, who often worked with Edna Walling, are also of note, as are photographs of houses by the architect Marcus Martin, who sometimes commissioned Edna Walling as landscape designer for his houses.