The Athenaeum's purpose, according to its organizational principles, is to collect materials "connected with the history and antiquities of America, and the useful arts, and generally to disseminate useful knowledge" for public benefit.

[2][5] It is presently a museum furnished with American fine and decorative arts from the first half of the 19th century.

In 2019, the Athenaeum of Philadelphia entered into an agreement with the libraries of the University of Pennsylvania to integrate their two collections, giving borrowing privilege to each other's patrons and making the Athenaeum's collection, which is focused on architecture, the built environment, and the decorative arts, searchable in Penn's online catalog.

It is awarded to authors who are "bona fide residents of Philadelphia or Pennsylvania living within a radius of 30 miles of City Hall".

[7] Eligible works are of general fiction or non-fiction; technical, scientific, and juvenile books are not included.