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Muriel Smith began her career as an Assistant Warden and Youth Leader of a purpose-built community centre outside Reading. In 1942 she trained in social work at Liverpool University and attended Reading University part time where she completed a degree in Philosophy and Psychology.
From 1949 to 1969 Muriel Smith worked with the London Voluntary Service Council (LCSS) as the head of the Community Development Department and was involved in the administering of grants from the LCC and GLC. She was also involved with the Central Housing Advisory Committee and a member of the Parker Morris Subcommittee which produced the report Homes for Today and Tomorrow. Her work brought her in touch with some of the major charitable trusts, in particular the City Parochial Foundation and the Gulbenkian Foundation in which Muriel was a member of many committees leading to various Gulbenkian publications.
In 1969 Muriel Smith was seconded to the Home Office as a consultant to the Community Development Project which was "...an attempt to research into the better understanding and comprehensive tackling of social needs, especially in local communities within older urban areas, through closer co-ordination of central and local official and unofficial effort, informed and stimulated by citizen initiative and involvement.", and later to the Voluntary Service Unit.
Muriel Smith was involved with the setting up of the Association of London Housing Estates and the Kenilworth Group.
Even after her retirement in 1979 Muriel Smith continued to be active in social work. She was responsible for three long-term Manpower Service projects, one sponsored by Toynbee Hall, were she helped with the preparations for their centenary year and gave a years voluntary service at their social centre working with mainly Bengali and Somali mothers and babies. The other two projects were sponsored by members of the Bengali local community who elected her as their organising secretary, as well as being a member of the Tower Hamlets Association for Racial Equality, and the subcommittee on education.