Smith has appeared on Broadway in the world premiere of Oslo,[2] the original American company of War Horse,[3] both at Lincoln Center, and in the 2009 revival of Equus[4] opposite Daniel Radcliffe and Richard Griffiths.

Other work in NYC includes the world premieres of plays by Richard Foreman, David Greenspan, Katori Hall and Anne Washburn, and in Sarah Ruhl’s Passion Play and Dead Man's Cell Phone.

Regional theatre work includes world premiere productions of plays by Sarah Ruhl, Mary Kathryn Nagle, Charles Mee, Tanya Barfield, Doug Wright, work with Theatre of War, and the 2007 collaboration[5] with artist/activist Paul Chan, The Classical Theatre of Harlem, and the public-arts presenters Creative Time to perform Samuel Beckett's play Waiting for Godot in the outdoor areas of New Orleans which had been most devastated by Hurricane Katrina.

Video of the production and Chan’s set pieces[6] are in the permanent collection at MOMA.

He supplies the voices of Baron Ünderbheit and Otto Aquarius on the cartoon TV series The Venture Bros., the voice of Sander Cohen in the videogame BioShock, (and the BioShock Infinite DLC Burial at Sea) and appears in the annual Bloomsday readings of James Joyce's novel Ulysses on Pacifica radio station WBAI.