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Employment to the National Library
In 1878, shortly after graduating university, Thomas Lyster officially joined the National Library of Ireland, and would be appointed assistant librarian at only twenty-three years of age. In 1895 Lyster would succeed William Archer as head librarian in 1895, until his retirement in 1920.

Career in the National Library of Ireland
During his time within the National Library, Lyster would become a strong advocate for the Dewey Classification System, increasing accessibility of the libraries inventory to the public. Lyster would permit students to access the classified collection within the library, as well as making periodicals available at the library counter, increasing readership numbers dramatically. Lyster would later endorse reading materials for young children, providing them with designated spaces in the library, with books on topics such as poetry, geography, and science. Furthermore, Lyster’s pragmatic and positive attitude would draw the attention of various readers from the library, many of which would seek his advice and assistance. Renowned Irish author W.B. Yeats would remark that Thomas Lyster had initially encouraged him to write, and would describe him as the most zealous man he’d known.

Library Association of Ireland
Thomas Lyster would go on to play a pivotal role in the establishment of the Cumann na Leabharlann (The Library Association of Ireland) and the Irish Rural Libraries Association. Lyster would later be elected as the organisation's vice-president in 1899, and begin a series of public lectures advocating for the expansion of the public library system. The Library Association would be established in 1904, with the aim to promote the establishment of public libraries. In 1904, Lyster would object that it was not a pertinent time for an organisation such as this to be created, however did voice his support for the eventual creation of an organisation in the future. Later that year, Lyster would become vice president of the organisation. Thomas Lyster would continue to serve as director of the National Library of Ireland until his retirement from the organisation in 1920.