The University’s administration building was completed in 1949 and named Sampson Hall in honor of Oscar R. Sampson. The Library was located in one wing of the building with a seating capacity of 100 and the capacity to hold 45,000 volumes. At the time, the Library had 138 periodicals, approximately 17,000 volumes, and a staff of 2. In May 1963, the library wing of Sampson Hall was named in honor of Miss Mary Hoyland Livermore. The Library remained in Sampson Hall until 1967 when a new building was constructed. This Library was known as Mary Livermore Library.

By the end of 1990, the Library contained approximately 180,000 volumes and 1,100 periodical subscriptions. The staff had increased to 21. A new administration building was constructed in 1995 and Sampson Hall was torn down to make room for the new addition to the Library. The name of the library building was officially changed to Sampson-Livermore Library on April 22, 1998.

The renovation included a two-story great hall with a glass ceiling, an electronic classroom for bibliographic instruction, a special collections room, a renovated computer lab, and additional office space. Library holdings increased to nearly 250,000 catalogued volumes, more than 400 electronic titles, and more than 1,300 print subscriptions. The Library also houses the most impressive collection of Lumbee Indian papers and materials in the country.

Currently, the Library provides an updated computer lab, multimedia and study rooms wired for network access, an up-to-date electronic reference center, and 24/7 access to electronic resources. On July 16, 2007, the Library was renamed Mary Livermore Library.