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The Silver Center of Arts and Science was built to replace New York University 's original Main Building. The Building replaced NYU's Old Main, a Town, Davis & Dakin's Gothic Revival structure constructed 1835-7; the use of prison labor from Sing-Sing sparked the Stonecutter's Riot in 1834, the first labor riot in NYC. In the old building, Samuel Colt developed the Revolver and Samuel Morse invented the Telegraph ; John William Draper in 1840 took one of the first photographs of a person on the roof. Walt Whitman taught poetry here, Winslow Homer painted here, and architects Alexander Jackson Davis and Richard Morris Hunt had offices here.

In addition to serving as the home of the College of Arts & Sciences, the light brick, stone and terra-cotta edifice also used to house portions the schools of commerce, law, and pedagogy as well as the offices of the American Book Company . This combination of institutional and commercial tenants is apparent in the building's tripartite facade design. The presence of the University on the three top floors is marked by engaged Ionic columns capped by Pediment s.

In 1927, due to the pressures of a growing post-war student body, NYU took over the entire building. Main Building became the home of NYU's Washington Square College until the University returned to Washington Square after giving up its second Bronx Campus in 1972, and the merger of University Heights and Washington Square colleges created CAS. Main Building was renamed the "Silver Center" in 2002 after Julius Silver, an alumnus of NYU, bequested $150 million to the university.