Matt’s first theatre roles came as part of the National Youth Theatre where he played Thomas Becket in Murder in the Cathedral at Westminster Cathedral, in front of an audience that included members of the government and royal family. He was Basoon in The Master and Margarita. This role earned him an agent and his first professional jobs. One of these was Fresh Kills opposite Christian Slater; and a short time later in On the Shore of the Wide World. During his tenure in On the Shore of the Wild World, the play transferred to the Royal National Theatre in London. When that closed, he took on the role of Lockwood, a pupil in the Alan Bennett play The History Boys.
His next role was the teen play Burn/Chatroom/Citizenship, and then Swimming with Sharks, his West End début, once again alongside Christian Slater.
Swimming With Sharks In 2007, Matt appeared as Henry in the critically acclaimed Polly Stenham play That Face at the Royal Court Theatre Upstairs in Chelsea alongside Lindsay Duncan as Henry's alcoholic mother, Martha, and Felicity Jones—later Hannah Murray—as Henry's drug-addicted sister, Mia. The play transferred to the Duke of York's Theatre in the West End in 2008 and became Matt's second role there. That Face focuses primarily upon alcohol and drug addiction in an upper-middle-class family after the paternal figure in the family leaves. As Henry, Smith portrayed an aspiring artist who left school to take care of his mother. To prepare for the role, the cast interviewed alcoholics and their family. Smith discussed his character's relationship with his mother in an interview with the Evening Standard:
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