As a legislator he promoted the Parliamentary Library. He organised the Governor, Sir Charles Hotham, to lay the foundation stones of University of Melbourne, Melbourne Public Library and Sunbury Industrial School [later Sunbury Lunatic Asylum] in 1854 – all on the same day. Sir Redmond Barry virtually single-handedly planned the Melbourne Public Library building and its contents. He had a 'hands-on' approach personally writing book selection and acquisition procedures – even to getting his hands dirty shelving books for the Library's 1856 opening. In 1862 and 1877-78 he went to Europe, England and America, purchasing books and pictures for University, Law and Public Libraries and Art Gallery. As Board of Trustees Chairman he was responsible for starting travelling libraries and supporting extended library hours. In September 1870 he "acquired" Marcus Clarke as Public Library Trustees clerk (later secretary), who until his death in 1881 worked as sub-librarian. "There can be fewer men with greater concern for and a greater and better vision for the young colonial society in which Redmond Barry made his life". Books and reading were intrinsic to Barry's own educational and intellectual development so he wanted these advantages for other people. The reason for his support of the Melbourne Public Library, the Law Library and his support of Mechanic Institutes was free access to libraries for all not just a select few. Barry never married, but had four children to Louisa Barrow, all of whom he acknowledged and supported. "The Argus" reported Sir Redmond Barry had been suffering from diabetes for about 10 years, but on his return from his trip to Europe and America it was apparent that the disease had affected his system. On Monday, 15 November, he was first troubled with the carbuncle on his neck. Sir Redmond was counselled by his medical adviser to at once rest from duty, but he was reluctant to do so, and continued to attend the court until he was compelled to take rest. He was constantly attended by Dr. Gunst, who however, could scarcely impress his patient with a sense of the very serious nature of his disease, which he regarded somewhat lightly. He became restless, and it was deemed advisable to place him under the constant care of a nurse. Despite the precautions, Barry caught cold through exposure, and congestion of the left lung set in. Dr. Gunst held a consultation with Dr. Teague, and pronounced the case hopeless. The left lung had become greatly congested, and this, together with the exhaustion and wasting away of the system resulting from the previous disease, proved fatal.