The idea of building a library as a memorial to the Mount Allison students who had died during the First World War was first proposed in 1917. Fundraising for the Memorial Library began after the Armistice in 1918, but construction did not start until 1926. The memorial was paid in part with money collected by donations from friends and family of the students and alumni. It was designed by Architect Andrew R. Cobb and formally opened on June 8, 1927.
The building's memorial hall displayed tablets with the names of the fallen soldiers from the First World War - the Mount Allison University First World War Tablet and Mount Allison Academy First World War Tablet.
In 1960, the architectural firm of C.A. Fowler & Company was enlisted to build an annex which connected to the main body of the Memorial Library with a large atrium. The Memorial Library building received extensive renovations in 1970, reopened in March 1971 and was demolished in December of 2011.