He began studying scientific subjects and chemistry in particular, in 1891 was appointed a laboratory assistant at the museum, and in the same year his first original paper was published in the Proceedings of the Linnean Society of New South Wales.
He became mineralogist at the museum in 1895, and in the same year in collaboration with Joseph Maiden contributed a paper on "Eucalyptus Kinos and the Occurrence of Endesmia" to the Proceedings of the Royal Society of New South Wales.
This was Smith's first contribution to organic chemistry; later on from 1898 to 1911 he lectured on this subject to evening students at the Sydney technical college.
[1] In 1896 he began his collaboration with Richard Thomas Baker with an investigation into the essential oils of the Sydney peppermint (Eucalyptus piperita).
Smith had been appointed assistant curator and economic chemist at the Sydney technological museum in 1899 and held this position until his retirement in 1921.