The actor will read poetry on the programme which is designed to encourage the joys of literacy in youngsters.
He said: "I've always had an enthusiasm for poetry and creative writing, having studied it at university, and as an actor it is so vital to my art to have an understanding and appreciation for classic literature."
Matt said the series offered "a whole new generation of young minds a way of learning and sharing poetry, and the fact that it's set to some of the most iconic Disney animations just makes the whole experience so enjoyable".
Smith will read Jack Prelutsky's Once They All Believed In Dragons in the second series of the programme, which also features David Walliams (Doctor Who), Jessica Hynes (Doctor Who) and Richard Briers (Doctor Who, Torchwood).
A Poem Is starts on 30th April, Disney Junior UK, at 5.25pm.
(Source: Press Association)