Though there was discussion of a national library for Wales in the 18th century, it was not until 1873 that a serious attempt began. Welsh material was collected and stored at Aberystwyth University College by a committee.

Members of Parliament and notable Welsh people battled tooth and nail to establish a National Library and a National Museum in Wales. In 1905, the government promised funds in its budget, and the Privy Council created a committee to choose the locations of the two institutes. Because the College already had a collection, Aberystwyth was chosen as the location for the Library. Sir John Williams, a physician and book collector, had also indicated that if the Library in Aberystwyth was completed, he would contribute his whole library to it. Because of its location in Cardiff, the National Museum was chosen.