"Captain America: Winter Soldier" star Sebastian Stan and 'The Office" alum Clark Duke have also signed on for the series, said The Hollywood Reporter.
The hour-long drama focuses on LA's celebrated and infamous stand-up comedy scene of the 1970s.
The pilot will delve into the inspired yet damaged psyches that inhabit the hilarious yet complex business of making an audience laugh.
Leo, 55, will play Goldie, a brassy comedy club owner who rules over her business with an iron fist and nurtures her comedians with tough love.
Stan, 33, will portray Clay, a funny, charming comedian on the rise whose biggest fear is irrelevancy. He is idolised by his ex and fellow comedian Cassie (Ari Graynor).
Duke, 30, has been cast as Larry, a ballsy young comedian from Boston who moves to LA with the hopes of making it big.
If picked up to series, Leo and Duke would be series regulars, while Stan would guest-star.
They join previously announced cast members Graynor, Erik Griffin, Andrew Santino, RJ Cyler and Stephen Guarino.
Carrey and Flebotte will executive produce alongside Michael Aguilar (The Departed) and Christina Wayne (Copper) for Endemol Shine Studios and Assembly Entertainment.
Jonathan Levine ('Warm Bodies') will helm the pilot.
The dramedy is based on the novel by William Knoedelseder.
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