Rosario Dawson, Brian Cox and Michael Wincott will lend their vocals to the series revivial.
Dawson will portray Lily Drawl, described as the "rising star" of the game's EuroCorp organisation. Cox has been cast as Jack Denham, a "ruthless power" behind the fictional firm's boardroom, while Wincott will play a senior agent named Jules Merit.
"I'm amazed how video games have become so deep in story, delivering fantastic worlds and memorable characters rivalling big Hollywood films," said Dawson.
"I was excited when EA approached me to play Lily Drawl in Syndicate. She's an interesting and strong female character. How cool is it to play the mastermind who designed the military chip inside the player's head?"
Syndicate is released for Xbox 360, PC and PlayStation 3 on February 21 in North America and February 24 in Europe.
> Read Digital Spy's review of Syndicate's co-op mode
> Read Digital Spy's interview with Syndicate executive producer Jeff Gamon
Watch a trailer for Syndicate below: