Answer by Foobie. Confidence votes 74. The largest library in the world is the U.S. Library of Congress in Washington, D.C. The British Library the world's other great library houses a collection comprising of 150 million items as against the 130 million housed by the Library of Congress.n terms of volume, the largest library in the Phillippines is the Central Philippine University Library. It has a collection containing more than 200,000 volumes, including b … ooks, journals, newspapers, magazines, maps, rare books, atlases, microforms, United Nations Documents, and sacred music.