Preparations for a University Library began in 1964 with the hiring of Donald Baird as University Librarian. The Burnaby campus was still under construction so the Library was set up in Vancouver at the BC Tel Building on Wylie Street under the Cambie Street Bridge. Baird began by obtaining copies of library book lists developed by new state universities in California and they served as the basis for SFU's collection. By the fall of 1965, the Library had 42 employees (12 of whom were librarians) who had catalogued and prepared 13,000 volumes for the new Library.

When the Library opened in September 1965 it served as a multi-purpose building with tenants that included administrative departments along with the Registrar's Office and the Office of the President. The first phase of the Library had 5 floors - the subject divisions were decentralized by floors and each floor had its own specialized subject information staff.

The earliest organization of the Library included a Processing Division and three Collections Divisions - Humanities, Social Sciences, and Sciences. By 1966 the Processing Division grew to five sections: Searching, Acquisitions, Cataloguing, Serials, and Government Publications and the Collections Division increased to four sections: Bibliographic Services, the Social Science Collection, the Humanities Collection, and the Science Collection. Two Assistant University Librarians were hired to oversee the Processing Division and the Collections Division and they reported to the University Librarian, who in turn, reported directly to the President until 1970. The Library also promoted an emphasis on automation that resulted in the formation of the (Information) Systems Division. In 1966, the University's Audio-Visual Services began in the Library.

The 1970s were a time of administrative and operational growth for the Library. During this time (1970-1979), the University Librarian reported to the Vice-President, Academic. By 1970 there were four Assistant Librarians, each heading a division – Processing, Collections, Information Systems, and the Audio Visual Centre. In late 1970 an ad hoc committee met to examine the concept of Special Collections and Archives that had been steadily growing as part of the Library's holdings. The Archives, established in 1968, functioned within the Special Collections Division of the Library. Various members of the library staff carried out archival duties. By the end of 1971 the university's administrative offices had moved out of the Library and the Library took on the operating responsibility for the University Bookstore. In 1973 the Audio Visual Centre moved out of the Library and in 1974, the Information Systems Division was replaced by the Planning and Budgeting Division. By 1978, the University Archives had become a separate administrative unit outside of the Library. That same year Baird retired as University Librarian and became University Archivist, a position he would hold until his retirement in 1990. Theodore (Ted) Dobb, previously serving as Deputy Librarian, was appointed the new University Librarian.

From 1979 until 1985, the University Librarian reported to the Associate Vice-President, Academic. In 1982 the Library was renamed the W.A.C. Bennett Library in recognition of the strong role that Bennett, former Premier of B.C., had in the creation of SFU. In 1985, the Library added a Reference Division and the Collections Division was renamed the Collections Management Office. From 1985 to 1990, Dobb reported to the Vice-President, Research and Information Systems. In 1990, the Librarian was again reporting directly to the Vice-President, Academic until 1994. That year, Paul Baldwin was appointed Associate Librarian, a position he held until 2002.

By 1991, the Library had grown to ten Divisions: Reference, Monographs, Collections Management, Serials, Loans, Systems, Support Services, Building, Belzberg Library, and the Bookstore. The heads of these divisions, as well as an Associate Librarian and Library Secretary reported to the University Librarian. In 1994, the Librarian began reporting directly to the renamed Vice-President, Research.

In 1998 Lynn Copeland replaced Ted Dobb as the new University Librarian. In 2005, Copeland was reappointed as University Librarian and Dean of Library Services.