Miller's production is unique among live-action Alice films in that he consciously avoided the standard Tenniel-inspired costume design and "florid" production values. Most of the Wonderland characters are played by actors in standard Victorian dress, with a real cat used to represent the Cheshire Cat. Miller justified his approach as an attempt to return to what he perceived as the essence of the story: "Once you take the animal heads off, you begin to see what it's all about. A small child, surrounded by hurrying, worried people, thinking 'Is that what being grown up is like?'"
The play featured a number of then-prominent British actors including Michael Redgrave (as the Caterpillar), John Gielgud (as the Mock Turtle),and Peter Sellers (as the King of Hearts), as well as two of Miller's fellow cast members from Beyond the Fringe, Peter Cook and Alan Bennett as the Mad Hatter and the Mouse, respectively. The title role was played by Anne-Marie Mallik, the 13-year-old daughter of a Surrey barrister, this being her only known acting performance. Wilfrid Brambell played the White Rabbit, Michael Gough and Wilfrid Lawson were the March Hare and the Dormouse, Alison Leggatt was the Queen of Hearts, and Leo McKern did a drag turn as the Ugly Duchess. The journalist and broadcasting personality Malcolm Muggeridge was The Gryphon. John Bird played the Fish Footman. The play also featured a young Eric Idle, several years before Monty Python brought him notice, uncredited as a member of the Caucus Race. David Battley appears briefly as the Executioner.
Interior scenes were shot at Netley Hospital, a mid-19th-century building that was demolished not long after the film was made.
The courtroom scene was shot at the BBC's Ealing Studios and involved the building of the largest set that Stage 2 at Ealing had ever seen.
Ravi Shankar wrote the music for the production, which was first broadcast on 28 December 1966.
- Director Jonathan Miller explained that the reason that none of the actors (even those playing non-human characters) wore costumes aside from Victorian period dress, was that he thought it was ridiculous to get big name stars to play parts (as he did in this version of Alice and MGM had done in their 1933 film version) and then cover them up in big costume animal heads so they were unrecognizable.
- Most of this show was shot with a 9mm camera lens.
- All the big name stars acted in this program for scale.
- Sir Ralph Richardson was offered a major cameo.
- Director Jonathan Miller chose Anne-Marie Mallik to play Alice because she had an appropriate sense of Victorian solemnity about her.