[5][6] While in the group, he directed and animated Victoria's Rocking Horse (1962), The Knight and the Fool (1963) and The Cage (1965), the first of which was the most celebrated of Amateur Cine World's Ten Best of 1962 and described by then secretary of the BFI, Stanley Reed as "extremley elegant.
[8] He was put to work on a wide range of projects including film titles for The Liquidator (1965), A Funny Thing Happened on the Way to the Forum (1966), Casino Royale (1967), and The Charge of the Light Brigade (1968).
[9] Le Cain turned freelance in 1969, working on sets for BBC television productions, continuing with animation projects, and beginning his career as a children's book illustrator.
His animation work for the BBC began with a production of Hans Christian Andersen's The Snow Queen, first broadcast on BBC2 on Christmas Day 1976, using live actors over backdrops designed by Le Cain.
[11] According to Phyllis Hunt, Le Cain's long-term editor at Faber, the major part of his time was spent on his animation work and he regarded his children's books "as holidays".
[14] Le Cain wrote 3 and illustrated 48 children's books during his lifetime,[15] recognised for their richly decorative watercolours and masterful command of design and colour.