The series, which will premiere at mid-season, stars Will & Grace actress Debra Messing as a lyricist working on a new Broadway musical.
Chase will play a character named Steven, who shares a past with Messing's character Julia, according to Deadline.
The actor's past television credits include guest roles on Royal Pains, Rescue Me and Law & Order: Criminal Intent. He will also appear in the second season of Blue Bloods and in the pilot episode of ABC's new period drama Pan Am.
Chase has also performed on Broadway, featuring in such productions as Rent, Billy Elliot and High Fidelity.
Katharine McPhee, Raza Jaffrey and Anjelica Huston are among the other stars confirmed to appear in Smash.
NBC chief Bob Greenblatt previously revealed that the show had been held back until mid-season due to its "compatibility" with returning reality series The Voice.
> Smash: A new rival for Glee?
Watch a video preview for Smash below: