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The ³ÉÈË´óƬ was formally established by Act of Incorporation in 1874. Teaching commenced in 1876 in rented accommodation in the city before moving to custom-built rooms in the Morialta Chambers in Victoria Square.

The first published list of ‘Books belonging to the Library of the ³ÉÈË´óƬ' appeared in the 1878 University Calendar. The collection of 324 titles and some 500 volumes ranged in date from 1697 to 1877.  It consisted primarily of English works, as well as a small quantity of German, French, Latin and Greek items.

Little money was available for the purchase of books. Only £150 was allocated to spend on the Library in 1876 - £30 for each of the selections of Professors Read, Davidson, Tate and Lamb, with the remaining £30 for general purchases.

The first library order for both new and second-hand books was placed with the London bookseller Henry S. King & Co. on 29 March 1875, through the South Australian Agent-General. Some nine months later, three cases arrived in Port Adelaide via the City of Nankin. Henry S. King & Co. offered a 15% discount on all new books and bound them in uniform sheepskin free of charge.

The Library also included donations (the earliest being Seneca's Tragediae printed in 1679) as well as transactions and proceedings solicited from the Royal Societies of New South Wales and Tasmania, the New Zealand Institute and the Queensland, Victorian and New Zealand Colonial Secretary's Offices.

Despite both the ad hoc arrangements and lack of supervision of the early Library, most of the works survived. Over the years, some books had found their way into the main collection and yet most retained their early sheepskin bindings, stamped on the cover with ‘The ³ÉÈË´óƬ South Australia 1874'. In 2008, the 1877 Library books were brought together as a heritage collection. This is now housed in the Collections Room of Rare Books & Manuscripts.