Smith received a BSc and PhD in chemistry at University of Canterbury in Christchurch, New Zealand before postdoctoral work at University of California, Berkeley (1991-1993) and the University of Göttingen (Humboldt Fellow 1989–1991).
In 1993 he started work at the University of Queensland, eventually heading up the Computational Reaction Dynamics Group before moving on to Oak Ridge National Laboratory in 2011 where he was the director of the Center for Nanophase Materials Sciences. After leaving Oak Ridge in 2017 Smith moved to the University of New South Wales where he founded the Integrated Materials Design Centre.
Smith left the University of New South Wales at the end of 2017 to become director of NCI Australia and professor of computational nanomaterials science and technology at Australian National University.