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With 1.3 million items, Smith has the largest undergraduate library system of any American liberal arts college. William Allan Neilson Library is the main library for the Smith campus and for graduate students. Neilson also includes an extensive Media Services Center (with films and videos) and two nationally prominent collections of rare books and women's history manuscripts. Young Science Library is one of the largest college science libraries in the country. Werner Josten Library for the Performing Arts has more than 52,000 recordings, a wide assortment of scripts and musical scores as well as books on theater, dance and music history. Hillyer Art Library holds a remarkable collection of art books and mounted photographs of works of art, maps and other visual materials.

Through an exchange with the Five College Consortium, Smith students also have access to the library holdings at Amherst, Mount Holyoke and Hampshire colleges and the University of Massachusetts' flagship campus in Amherst.