[4] Smith's early acting experience started in 1925 when he was one of the founders of the Harvard University Players, which later included Henry Fonda, James Stewart, Joshua Logan and Margaret Sullavan in Falmouth, Massachusetts.

He continued acting in films such as Comanche (1956); Sayonara (1957); Party Girl (1958); The Mugger (1958); Imitation General (1958); The Badlanders (1958); This Earth Is Mine (1959); Strangers When We Meet (1960); Susan Slade (1961); The Balcony (1963); A Distant Trumpet (1964); Youngblood Hawke (1964); The Young Lovers (1964); The Trouble with Angels (1966); A Covenant with Death (1967); Games (1967); The Money Jungle (1968); Kona Coast (1968); Assignment to Kill (1968); Death of a Gunfighter (1969); The Games (1970); Pete 'n' Tillie (1972); Die Sister, Die!

During World War II, Smith served as a private in the U.S. Army, making training films covering among others, medical, dental, artillery, and electronics.

[7]: 831 Smith had roles in TV movies such as How Awful About Allan (1970), The Night Stalker (1972), The Judge and Jake Wyler (1972), The Cat Creature (1973), The Affair (1973) and The Disappearance of Flight 412 (1974).

He began guest-starring in television series in 1949 in The Philco Television Playhouse and appeared in Robert Montgomery Presents; General Electric Theater; Alfred Hitchcock Presents; Naked City; Have Gun – Will Travel; Perry Mason; Gunsmoke “Beaton” (1963), a man trying to steal two Irish immigrants’ land in “Two of a Kind” (S8E27, 1963), "Dakota" (1963), and as an aging gunslinger in “The Glory & The Mud” (S9E14); The Beverly Hillbillies; Rawhide S2 E8 as Capt.