Emms told CultBox that he wants the former Doctor Who star to play the mythical character of Icarus on the BBC's family fantasy series.
"We'd love to have someone like Matt Smith come in," said Emms, who plays Pythagoras on the show.
"I know we were all wondering if they're going to do the Icarus story at some point [and] he'd be brilliant as Icarus."
Atlantis previously introduced Robert Lindsay as fabled Greek inventor Daedalus - the father of Icarus.
"I know there were talks about Robert coming back," Emms confirmed. "I'd love him to come back."
Atlantis was renewed for a second series back in October, with BBC One controller Charlotte Moore branding the show an "original British drama with the kind of scale and ambition that we've come to expect from the cinema".
Atlantis: What do you want from a second series?