The 'Battlestar Galactica' actor will play Robert Gonzales, a mysterious character whose arrival promises to have "massive repercussions for Director Coulson and his team."
Marvel.Com added that he will debut in March when 'Agents of SHIELD' returns.
Executive Producer and Marvel's Head of Marvel Television Jeph Loeb said: "Edward James Olmos brings an amazing gravitas to any role he inhabits, something we knew we needed for Robert Gonzales.
"When Olmos first appears on our series, everyone will have to take notice - including our favourite Agents."
Blair Underwood is joining the cast for the new season as well.