[1][2] Shortly following his graduation from the EMA Higher Drama School in 2002, Mart Toome began an engagement as an actor at the Tallinn City Theatre, where he is still currently employed.

Some of his most memorable roles since joining the Tallinn City Theatre include those in stage productions by such varied international playwrights and authors as: Shakespeare, Dostoyevsky, Yeats, Dumas, Chekhov, Steinbeck, Waugh, Ferenc Molnár, Aleksey Nikolayevich Tolstoy, David Mamet, Sławomir Mrożek, Carlo Gozzi, Ann Jellicoe, Tennessee Williams, J.

Among his more memorable performances in roles by Estonian playwrights and authors include those of: Eduard Vilde, A. H. Tammsaare, Jaan Tätte, Diana Leesalu, and Paavo Piik.

[9] Toome took Ardo Ran Varres's place in the Estonian language dubbing of the Nickelodeon animated television series SpongeBob SquarePants, or Käsna-Kalle Kantpüks, starting with the show's seventh season.

In 2005, he appeared in a small role in the Peeter Urbla directed comedy-drama Stiilipidu for Exitfilm about three women (played by Maarja Jakobson, Anne Reemann, and Evelin Võigemast) who lose their jobs and open a costume rental business.