Smethurst made his film debut in 1958's Carry On Sergeant. This was followed by parts in the films Saturday Night and Sunday Morning (1960), A Kind of Loving (1962), Run with the Wind (1966), Night After Night After Night (1970), the big-screen version of Please Sir! (1971) and the ITV sitcom For the Love of Ada (1970–71) amongst others, before he landed the role for which he is best known – that of bigoted socialist and union leader, 'brother' Eddie Booth in Love Thy Neighbour. The programme ran for eight series between 1972–76. During this run he also appeared in the 1974 film version of the sitcom Man About the House.