Walker accepted the presidency of the Massachusetts Institute of Technology in 1881, a position he held for fifteen years until his death. During his tenure, he placed the institution on more stable financial footing by aggressively fund-raising and securing grants from the Massachusetts government, implemented many curricular reforms, oversaw the launch of new academic programs, and expanded the size of the Boston campus, faculty, and student enrollments. MIT's Walker Memorial Hall, a former students' clubhouse and one of the original buildings on the Charles River campus, was dedicated to him in 1916.