His father was a prominent local businessman, holding executive positions at the Franklin Iron Works, Clinton Bank, and the company that managed the Niagara Falls Suspension Bridge.

[5] On July 30, 1891, the younger Charles Smyth married Ruth Anne Phelps, originally of Shreveport, Louisiana.

He became interested in geology at a young age: his native region of Upstate New York had many fossils, and his family's business involved extracting the local iron ore.

He then spent an additional year studying petrology at Heidelberg University under Harry Rosenbusch,[5] the world expert in the field.

[3] In addition to his teaching duties at Hamilton, Smyth spent each summer from 1892 to 1903 doing field work for the New York State Museum in the western Adirondack Mountains, which had been studied very little in the fifty years prior.

He collaborated with his old advisor Kemp, who specialized in the eastern Adirondacks, and Henry Platt Cushing, who claimed the northern and northeastern sections.

[8] He was also a member of the Society of Economic Geologists, the American Institute of Mining and Metallurgical Engineers, the Washington Academy of Sciences, Phi Beta Kappa, and Sigma Xi.

His Princeton graduate student Hayes proved a similar result about the iron ores of his native Wabana, Newfoundland and Labrador.

[5] Smyth, Kemp, and Cushing's field work in the Adirondacks yielded detailed geologic maps of the challenging region.

[5][8] In his later years Smyth suffered from poor health, which an obituary in Princeton Alumni Weekly blamed on "overwork in certain rugged inaccessible wilderness portions of the Adirondacks.