The drama focuses on a woman with a difficult past who moves to a small town in Maine, where the magic of fairytales appears to be real.
Deadline reports that Carlyle has signed up to play Rumpelstiltskin in the project.
The character is said to be an expert in dark magic who agrees to help Snow White and Prince Charming fight the Evil Queen's spells.
Carlyle played Dr Nicholas Rush in Stargate Universe until it was cancelled in December. He has also appeared in movies such as The Full Monty, Trainspotting and 28 Weeks Later.
Once Upon A Time has been penned by Tron: Legacy and Lost writers Edward Kitsis and Adam Horowitz.
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