- Dick Van Dyke
- Caractacus Potts
- Sally Ann Howes
- Truly Scrumptious
- Lionel Jeffries
- Grandpa Potts
- Gert Fröbe
- Baron Bomburst
- Anna Quayle
- Baroness Bomburst
- Benny Hill
- Toymaker
- James Robertson Justice
- Lord Scrumptious
- Robert Helpmann
- Child Catcher
- Heather Ripley
- Jemima
- Adrian Hall
- Jeremy
- Barbara Windsor
- Blonde
- Davy Kaye
- Admiral
- Alexander Doré
- First Spy
- Bernard Spear
- Second Spy
- Stanley Unwin
- Chancellor
- Peter Arne
- Captain of Guard
- Desmond Llewelyn
- Coggins
- Victor Maddern
- Junkman
- Arthur Mullard
- Big Man
- Ross Parker
- Chef
- Gerald Campion
- Minister
- Felix Felton
- Minister
- Monti DeLyle
- Minister
- Totti Truman Taylor
- Duchess
- Larry Taylor
- Lieutenant
- Max Bacon
- Orchestra Leader
- Max Wall
- Inventor
- John Heawood
- Inventor
- Michael Darbyshire
- Inventor
- Kenneth Waller
- Inventor
- Gerald Taylor
- Inventor
- Eddie Davis
- Inventor
- Robert Arditti
- Dancer
- Vic Armstrong
- Cavalry Guard at Cannon
- Michael Audreson
- Peter
- Theo Aygar
- 4th Minister
- John Baskcomb
- Castle Chef
- Roy Beck
- Grand Prix Spectator
- Jimmy Berriman
- Child in Castle
- Eunice Black
- Courtier
- Bill Brandon
- 'Test your Strength' Attendant
- Daniel Brown
- Townsman
- Phil Collins
- Vulgarian Child
- Tim Condren
- Cavalry Guard
- Sadie Corre
- Field Worker
- John Corrie
- Soldier
- John Crocker
- Under Chef
- Cyril Cross
- Minister
- Dan Darnelli
- Man in the Sweet Factory
- Gabrielle Daye
- Lady-in-Waiting
- Liz English
- (uncredited)
- Ernest Fennemore
- Man at Fair
- Harry Fielder
- Soldier at Castle
- Henry Gibson
- Dancer
- Gary Graham
- Child in Castle
- Carson Green
- Urchin
- Kay Hamilton
- 3rd Duchess
- Miranda Hampton
- Scullery Maid
- John Hicks
- Boy
- Robert Jenner
- Field Worker
- Nigel Kingsley
- Child in Castle
- Teddy Kiss Atom
- Minor Role
- George Leech
- Chitty's original driver
- Jim Machin
- Child
- Mary Maxfield
- Lady at the Fair
- Connel Miles
- Dancer
- Roy Murray
- Fairground Barker
- Grace Newcombe
- 2nd Duchess
- Dickie Owen
- Major Domo
- Paul Phillips
- Soldier
- Dido Plumb
- Townsman
- Colin Rix
- Chauffeur
- Jessie Robins
- Pastry Cook
- Joseph Ross
- Child in Castle
- Peter Ross
- Child in Castle
- Janette Rowsell
- Scullery Maid
- John Ruddock
- Minister of Finance
- Gary Smith
- Boy
- Hugh Spight
- Background
- Ian Spofforth
- Minor Role
- Reg Thomason
- Castle Guest
- Margot Travers
- Dancer
- Rosetta Tropea
- Child at the Fair
- Richard Wattis
- Secretary at Sweet Factory
- Jeannette Wild
- Minor Role
- Freddie Wilson
- Boy
- Bob Wright
- Grand Prix Official
