Additionally, he has guest-starred in Utopia, The Newsreader, Five Bedrooms, Underbelly: Fat Tony & Co., Wentworth, Mr & Mrs Murder, Play School, City Homicide, The Strange Calls, Temptation, and The Postcard Bandit.
He joined the original Australian cast of Jersey Boys, in the role of Franki Valli (Alternate), that same year, but left the production prematurely due to health complications.
[12] In 2010, he sang the role of Skeets Miller in a one-off concert performance of Adam Guettel's Floyd Collins at City Recital Hall in Sydney.
[13] Simpson-Deeks played the role of Constable Alexander Fitzpatrick in Ned: A New Australian Musical at Bendigo's Ulumbarra Theatre in 2015, and is featured on the show's Official Cast Recording.
Simpson-Deeks created the character of Daniel "Danno" Bookham for the popular educational video game Murder Under the Microscope, and played the role from 2007 to 2012.