Following another sixteen–month stint as Shane Swanson on Hollyoaks (2005–07) which ended in January 2007 after Donoghue was axed, Donoghue was cast in the role of Dominic Pearce in the upcoming science-fiction television series Outlanders, making his first appearance as one of the six original protagonists in the series in the pilot episode.
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Shortly after departing Outlanders in November 2010 Donoghue announced that he would be returning to Hollyoaks in the new year in his third stint on the show.
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As a member of the cast Outlanders Donoghue has won a total of four British Academy Television Awards for Best Drama Series.
Other recurring enemies include Colonel Thrush, Sam the Imperator, Grigori Zakat and Maccan, the last prince of the Tuatha Dé Danann.