In 1970, Butler resigned from Imperial College and his active involvement in physical research ceased. He accepted the role of director of the Nuffield Foundation, a charitable foundation influential in education. During his time there he set up a group for research and innovation in higher education, a programme for law and society, and the centre for agricultural strategy at the University of Reading. His role in the establishment of the Open University was also important, since the Nuffield Foundation funded a course on genetics as a test bed for other courses. He was appointed to the council of the Open University in 1971 and stayed as a member until 1995, serving as vice-chairman from 1986 to 1995. In 1975, Butler was appointed vice-chancellor of Loughborough University, retaining that post until he retired in 1985.