After returning to Britain, Playfair became manager of a calico works in Primrose, near Clitheroe, and in 1843 was appointed Professor of Chemistry at the Royal Manchester Institution, where he was assisted by Robert Angus Smith. Two years later, he was made chemist to the Geological Survey, and subsequently became Professor in the new School of Mines. In 1848, he was elected to the Royal Society, and three years later was made Special Commissioner and a member of the executive committee of the Great Exhibition.