Jeremy Brett as Sherlock Holmes

Edward Hardwicke as Dr. John Watson

Raymond Adamson as Sir Charles Baskerville

Alastair Duncan as Dr. Mortimer

Ronald Pickup as Barrymore

Rosemary McHale as Mrs. Barrymore

Kristoffer Tabori as Sir Henry Baskerville

James Faulkner as Stapleton

Edward Romfourt as Purser

Philipp Dettmer as Pageboy

Stephen Tomlin as Perkins

Fiona Gillies as Beryl Stapleton

Bernard Horsfall as Frankland

Don McKillop as Vicar of Grimpen

William Ilkley as Selden

Myrtle Devenish as Postmistress

Elizabeth Spender as Laura Lyons

Donald Bisset as Manservant (uncredited)