[10] John Harvard was a Puritan minister who accumulated 400 books spreading word of his faith.

The works in this collection soon became obsolete, as Harvard Library quickly changed to an academic institute and found little need for the theological titles.

[12] Thomas Hollis V, great-nephew of one of the university's early benefactors, began shipping thousands of specially chosen volumes to the library.

[16] Harvard Library houses a range of historical artifacts and primary documents from around the world, including one of only 23 complete Gutenberg Bibles.

Botany Libraries’ archives include Henry David Thoreau’s personal herbaria, letters from Charles Darwin to Asa Gray, and thousands of botanical illustrations.

The Wolbach Library, which was established in 1975 and closed March 22 2024, held the oldest surviving images of the Moon.

[21] The CURIOSity tool offers another way to explore Harvard's digital collections, providing curated views, specialized search options and discovery of unique content.

Curated collections include the Colonial North America archive, the Islamic Heritage Project, and over 3,5000 digitized daguerreotypes.

[22] By 1973, Harvard Library had authored or published over 430 volumes in print in addition to nine periodicals and seven annual publications.

[24] Harvard Library is the formal name for an administrative entity within the central administration that oversees the development and implementation of strategies that facilitate access to research, collections, services, and space in ways that raise the value of the university's investment in its libraries.

As of June 2019[update], Martha Whitehead is the current vice president for Harvard Library and the Roy E. Larsen Librarian of the Faculty of Arts and Sciences.

Other members include representatives from the Tell Us project, the Berkman Institute, and Harvard Library Shared Services.