Mount Union shares the Innovative Interfaces catalog system with 23 OPAL libraries as well as 74 OhioLINK libraries throughout Ohio. The estate of Louis H. Brush provides annual grants to purchase books and periodicals in memory of James Alpheus Brush, the first Librarian of the University, and his wife. In 1971, the Thomas S. Brush Foundation, Inc. made a gift of approximately $500,000 to the University Endowment Fund to be used for purchase of books and periodicals in memory of Mr. Brush’s grandparents, Mr. and Mrs. Louis H. Brush.

The Sturgeon Music Library is located in Cope Music Hall. This facility was given in memory of Bertha Fogg Sturgeon and her parents, by Samuel Sturgeon. The collection of books, scores and recordings was begun by a generous donation by Mrs. Ella Wilcox Peasley and the Carnegie Corporation. Presently, there are more than 7,000 recordings in CD format, more than 10,000 music scores, a music reference collection, music and theatre DVDs, and music periodical titles in the library. In addition, the library houses Mount Union faculty and student performance recordings from 1956 to the present. The Sturgeon Music Library houses metronomes, tuners, stereos, and other electronics available for checkout. There is a selection of theatre titles for current coursework including plays, and technical books for stage and costumes. There are computer workstations and printer with access to the campus network, the library system, and the Internet.