The Wondercrump World of Roald Dahl opens in the Cardiff Bay venue on Friday and will run for 22 weeks.
It will feature original manuscripts and handwritten letters and will look at his life from Llandaff schoolboy to fighter pilot and author.
The 100th anniversary of Roald Dahl's birth will be marked on 13 September.
Cardiff is gearing up for weeks of events and exhibitions in honour of the author, who was born in the city.
The Wondercrump World of Roald Dahl opened earlier this year at the Southbank Centre in London and has now moved to Cardiff.
It will run until 14 January 2017 - the largest exhibition staged at the WMC to date.
Graeme Farrow, artistic director at the centre, said it was "fantastic" to welcome the event to the city of Dahl's birth.
"This magical exhibition allows you to explore Dahl's pure imagination and I have no doubt that Wondercump will inspire hundreds of young minds to go on to create wonderfully imaginative worlds of their own," he added.
It will feature artefacts from the Roald Dahl Museum and Story Centre in Great Missenden, Buckinghamshire, where the author lived and worked for over 35 years.
Director Steve Gardam said: "The Roald Dahl archive reveals the writer's craft behind the magic."
The Wondercrump World of Roald Dahl forms part of Roald Dahl 100, a year of celebration throughout 2016 marking 100 years since his birth.
An interactive exhibition inspired by Roald Dahl is opening at the Wales Millennium Centre, promising the chance to delve into the author's imagination.