The Smith family papers consist mostly of Alfred Smith's letters to his parents while he was in the Army, and correspondence exchanged by family members in Michigan and New York in the years following the war. The collection also includes various documents including insurance policies, deeds, mortgages, and a lottery advertisement (1868).

Subjects of particular interest from Alfred's correspondence include conditions in the Union hospital at Albany, New York (July 12, 1862); Smith's transfer from the Army of the Potomac in Virginia to the Army of the Cumberland in Tennessee (October 8, 1863); the Battle of Marietta, Georgia (July 13, 1864); and a scheme by "copperheads" to set up a Northwestern Confederacy (August 4, 1864). Alfred Smith also set forth his opinion on the necessity of abolishing slavery and disagreed with General McClellan's plan to allow the South back into the Union on the same footing as before the war (October 24, 1864). After the war, Alfred spent some time in Lansing, Michigan. His letters include a description of the new capitol building plans (March 10, 1872), and an account of his visit to the state legislature when Zachariah Chandler was elected to succeed U.S. Senator Isaac P. Christiancy (February 15, 1879).