Her television acting credits included "His and Hers", "The Steam Video Company", "Doctor in the House", "Clochemerle" and "The Two Ronnies" with Tim Brooke-Taylor. Actress was a member of the regular cast for the BBC2 series "The End of the Pier Show" (1974) and "In The Looking Glass" (1978), along with John Wells, John Fortune, and Carl Davis.

Though credited as 'Maddy Smith', Madeline Smith first worked for Hammer films in "Taste the Blood of Dracula" (1969), as an East End prostitute, a non-speaking role, just much child-like pouting. Her Hammer Heroine cult status derives primarily from "The Vampire Lovers" (1970) and "Frankenstein and the Monster from Hell" (1974).

Her portrayal of Bond girl Miss Caruso in the opening of "Live and Let Die" differs significantly from other renditions of Bond girls - while most actresses tend to portray Bond girls as cynical, world weary and knowing, Smith portrayed Miss Caruso, an Italian agent, as sweet, vulnerable and innocent, qualities generally not associated with Bond girls.