To pursue his goals—to begin in earnest his journey "up from slavery"—Washington needed to return to his home state. It was while working in a West Virginia salt mine that Washington first heard of the Hampton Institute in Hampton, Virginia. Founded in 1868, Hampton provided former slaves and their children greater opportunities than did smaller schools like the one Washington had been attending intermittently in West Virginia. In particular, it offered a chance at an "industrial education," which combined such traditional subjects as reading and geography with training in various manual arts (carpentry, bricklaying, and sewing, for example) as well as teacher training. Washington traveled to Hampton, covering much of the trip on foot and with little or no money, in 1872. When he arrived he was required to sweep and dust a room as an "exam"—a test he passed easily, disciplined as he had become through his work as a houseboy. According to Samuel Chapman Armstrong, Hampton's founder, Washington distinguished himself during his three years there as the best student the school had ever had. He graduated in 1875, returned to Malden to teach for three years, spent the winter of 1878–79 studying at the Wayland Seminary in Washington, D.C., then returned to Hampton Institute in 1879 to work for two years as a night-school teacher and a supervisor of the Kiowa and Cheyenne students recently accepted at the school.

Had he simply continued his career at Hampton, Washington could have viewed himself as an unqualified success. The chance to pursue something greater came quickly, however. In May 1881 Armstrong recommended him to head a new school for African Americans to be founded in Tuskegee, Alabama. The school opened two months later, on July 4. Its first class numbered only thirty students. Washington himself was the lone faculty member, and most of the teaching was done in a "little shanty" on loan from a Methodist church. By 1900 the student body numbered 1,100 and the faculty more than eighty. By the time of Washington's death in 1915, Tuskegee had enrolled 1,500 students for the year and its campus encompassed some 100 buildings and 3,500 acres.

Washington's personal life was difficult during these years, however, due to the poor health of his wives. He married his first wife, Fanny Norton Smith Washington, in 1882. She died two years later. His second wife, Olivia Davidson Washington, had been one of Tuskegee's most important fund-raisers prior to marrying Washington in 1885. She continued to perform that work until her death in 1889. Washington was survived by his third wife, Margaret Murray Washington, and by three children from his earlier marriages, all of whom did work for the institution.

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